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The first issue is scheduled to be published in Dec. 2018.
Call for Papers
CCS Chemistry is the flagship general journal for the cutting edge and fundamental research in the areas of chemica research facing global audiences published by Chinese Chemical Society. We call for excellent papers cover but not limited to synthetic chemistry, catalysis & surface chemistry, chemical theory and mechanism, chemical metrology, materials & energy chemistry, environmental chemistry, chemical biology, chemical engineering and industrial chemistry. Professional arrangement ensures that all papers can be reviewed and published online quickly and efficiently (one or two weeks).
Contact information:
Dr. Hao Linxiao, haolinxiao@iccas.ac.cn; +86-10-82449177-888
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2026, 37(4): 110726
doi: 10.1016/j.cclet.2024.110726
Abstract:
Rechargeable aqueous zinc-ion batteries (AZIBs) have received considerable attention in recent years because of their high safety, low cost, and environmental friendliness. The properties of cathode materials are vital for the further development of AZIBs. Graphene-based composite materials have emerged as promising cathode materials for AZIBs on account of their superior electrical conductivity and excellent electrochemical performance. Considering the rapidly progress of graphene-based composites, we comprehensively summarize the recent progress in the applications of graphene-based composites as the cathode in AZIBs. Furthermore, the relationships between their synthetic methods, nano- and microstructures, and electrochemical performance are systematically concluded and discussed. Finally, rational suggestions and prospects for the future development of graphene-based composites are also proposed.
Rechargeable aqueous zinc-ion batteries (AZIBs) have received considerable attention in recent years because of their high safety, low cost, and environmental friendliness. The properties of cathode materials are vital for the further development of AZIBs. Graphene-based composite materials have emerged as promising cathode materials for AZIBs on account of their superior electrical conductivity and excellent electrochemical performance. Considering the rapidly progress of graphene-based composites, we comprehensively summarize the recent progress in the applications of graphene-based composites as the cathode in AZIBs. Furthermore, the relationships between their synthetic methods, nano- and microstructures, and electrochemical performance are systematically concluded and discussed. Finally, rational suggestions and prospects for the future development of graphene-based composites are also proposed.
2026, 37(4): 110790
doi: 10.1016/j.cclet.2024.110790
Abstract:
Alkali metal-ion batteries, such as lithium-ion and sodium-ion batteries, have been widely recognized by both academia and industry for their high energy density, long cycle life, low self-discharge rate, and environmental friendliness. Theoretical calculations are crucial in elucidating the energy storage mechanism of alkali metal-ion batteries and in designing the next generation of high-performance energy storage systems. This article reviews the application of theoretical calculations in alkali metal-ion batteries. These calculations are instrumental for experimental researchers in understanding the microscopic design of electrode materials, optimizing various interfaces and electrolyte structures, and clarifying ion and electron transport behaviors as well as electrochemical reaction mechanisms. Specifically, researchers typically calculate the reduction reactions, charge state changes, and structural changes of cathode materials to predict their electrochemical reactivity and optimize their performance and stability. Calculations and simulations of alkali metal batteries focus on ion transport dynamics within the electrolyte, including energy level distribution, solvation structure, and molecular dynamics simulations. Analyzing oxidation reactions, ion diffusion, and volume changes in various alkali metal-ion battery anode materials enables the screening and design of new anode materials with superior electrochemical properties. This review also discusses the challenges of applying theoretical calculations in alkali metal-ion batteries and provides an outlook for future research. Critical insights are offered for advancing research paradigms that integrate theoretical and experimental approaches in the development of energy storage electrode materials.
Alkali metal-ion batteries, such as lithium-ion and sodium-ion batteries, have been widely recognized by both academia and industry for their high energy density, long cycle life, low self-discharge rate, and environmental friendliness. Theoretical calculations are crucial in elucidating the energy storage mechanism of alkali metal-ion batteries and in designing the next generation of high-performance energy storage systems. This article reviews the application of theoretical calculations in alkali metal-ion batteries. These calculations are instrumental for experimental researchers in understanding the microscopic design of electrode materials, optimizing various interfaces and electrolyte structures, and clarifying ion and electron transport behaviors as well as electrochemical reaction mechanisms. Specifically, researchers typically calculate the reduction reactions, charge state changes, and structural changes of cathode materials to predict their electrochemical reactivity and optimize their performance and stability. Calculations and simulations of alkali metal batteries focus on ion transport dynamics within the electrolyte, including energy level distribution, solvation structure, and molecular dynamics simulations. Analyzing oxidation reactions, ion diffusion, and volume changes in various alkali metal-ion battery anode materials enables the screening and design of new anode materials with superior electrochemical properties. This review also discusses the challenges of applying theoretical calculations in alkali metal-ion batteries and provides an outlook for future research. Critical insights are offered for advancing research paradigms that integrate theoretical and experimental approaches in the development of energy storage electrode materials.
2026, 37(4): 110791
doi: 10.1016/j.cclet.2024.110791
Abstract:
Chirality, a fundamental property of biological systems, is widely present at the molecular, cellular, and tissue levels. Current studies have shown that chiral inorganic nanomaterials, have good chiral optical activity as well as high enantioselectivity. When interacting with biological systems, the enantioselective behavior of chiral inorganic nanomaterials towards biomolecules can distinguish between different isomers of biomarkers, which, combined with the excellent optical activity of chiral inorganic nanomaterials, allows for the rapid and sensitive detection of biomarkers. Moreover, chiral inorganic nanomaterials exhibit stronger internalization and retention capabilities in cells, and by specifically targeting specific biomarkers can regulate cellular activity and catalyze related reactions, thereby achieving synergistic treatment of various diseases. In addition, chiral inorganic nanomaterials also have good biocompatibility and do not cause cell damage in living organisms. Moreover, chiral inorganic nanomaterials have programmable surfaces that can be tailored to suit specific biological functions. Due to the important role of chiral inorganic nanomaterials in the biomedical field, this paper summarizes and discusses the synthesis and biomedical applications of chiral inorganic nanomaterials. It further looks forward to its future development prospects to provide a reference for promoting relevant research on chiral inorganic nanomaterials in biomedical fields.
Chirality, a fundamental property of biological systems, is widely present at the molecular, cellular, and tissue levels. Current studies have shown that chiral inorganic nanomaterials, have good chiral optical activity as well as high enantioselectivity. When interacting with biological systems, the enantioselective behavior of chiral inorganic nanomaterials towards biomolecules can distinguish between different isomers of biomarkers, which, combined with the excellent optical activity of chiral inorganic nanomaterials, allows for the rapid and sensitive detection of biomarkers. Moreover, chiral inorganic nanomaterials exhibit stronger internalization and retention capabilities in cells, and by specifically targeting specific biomarkers can regulate cellular activity and catalyze related reactions, thereby achieving synergistic treatment of various diseases. In addition, chiral inorganic nanomaterials also have good biocompatibility and do not cause cell damage in living organisms. Moreover, chiral inorganic nanomaterials have programmable surfaces that can be tailored to suit specific biological functions. Due to the important role of chiral inorganic nanomaterials in the biomedical field, this paper summarizes and discusses the synthesis and biomedical applications of chiral inorganic nanomaterials. It further looks forward to its future development prospects to provide a reference for promoting relevant research on chiral inorganic nanomaterials in biomedical fields.
2026, 37(4): 110972
doi: 10.1016/j.cclet.2025.110972
Abstract:
With the increasing demand for high-energy-density lithium ion batteries, it has become increasingly imperative to address the safety concerns associated with batteries. At present, the design of flame-retardant electrolytes has been widely studied. However, most strategies lack the discussion of battery-level safety, and have only conducted primary safety tests such as ignition. In this situation, it is necessary to analyze the intrinsic link between flame-retardant electrolytes and battery safety. This paper elucidates the role of flame-retardant electrolytes in the thermal runaway process of batteries and proposes a strategy to enhance the safety of batteries from the aspect of electrolytes. Then the thermal, electrochemical and interfacial stability characteristics of different flame-retardant electrolytes are analyzed in detail based on their structures, and the basic principles for the design of their solvent structures are pointed out to enhance electrochemical performance. Furthermore, a prospective summary of safety characterization at the material and battery level is presented, aiming to build a comprehensive battery safety characterization system. This review provides insights into the design of flame-retardant electrolytes for high safety batteries.
With the increasing demand for high-energy-density lithium ion batteries, it has become increasingly imperative to address the safety concerns associated with batteries. At present, the design of flame-retardant electrolytes has been widely studied. However, most strategies lack the discussion of battery-level safety, and have only conducted primary safety tests such as ignition. In this situation, it is necessary to analyze the intrinsic link between flame-retardant electrolytes and battery safety. This paper elucidates the role of flame-retardant electrolytes in the thermal runaway process of batteries and proposes a strategy to enhance the safety of batteries from the aspect of electrolytes. Then the thermal, electrochemical and interfacial stability characteristics of different flame-retardant electrolytes are analyzed in detail based on their structures, and the basic principles for the design of their solvent structures are pointed out to enhance electrochemical performance. Furthermore, a prospective summary of safety characterization at the material and battery level is presented, aiming to build a comprehensive battery safety characterization system. This review provides insights into the design of flame-retardant electrolytes for high safety batteries.
2026, 37(4): 111013
doi: 10.1016/j.cclet.2025.111013
Abstract:
Traditional chemotherapeutic approaches lack selectivity and damage both cancerous and healthy cells. In contrast, cancer immunotherapy harnesses the host's immune system to selectively target and eradicate tumor cells, offering tremendous potential for the long-term suppression of tumor growth and preventing its recurrence. However, tumors often develop immune evasion by exploiting immune checkpoints, which regulate the immune system. Among these checkpoints, programmed death protein 1 (PD-1) and its ligand (PD-L1) have garnered significant interest because they play a key role in protecting the tumor cells from immune-mediated eradication. The approval of monoclonal antibodies (mAbs) that target PD-1/PD-L1 by the Food and Drug Administration (FDA) is a milestone in immunotherapy. Although mAbs have demonstrated remarkable success in treating skin melanomas, their efficacy against other solid tumors remains limited. There is a clear need to explore new approaches to enhance the efficacy of mAbs and find more effective checkpoint inhibitors. Metal-based drugs offer a new platform to address this challenge. This review highlights the recent progress in leveraging metal complexes as PD-1/PD-L1 inhibitors. We discussed metal-based agents used either alone or in combination with mAbs to boost the immune system. We also highlighted examples of metallodrugs encapsulated within the nanoparticles to augment the efficacy of immune checkpoint therapy. While research on metal-based complexes targeting PD-1/PD-L1 is still in its infancy, the examples presented here will serve as the basis for future discussions and efforts in this emerging field. We anticipate that ongoing research in targeting immune checkpoint blockade with innovative metal-based therapeutics will enhance the scope of treatment across a wide range of cancers.
Traditional chemotherapeutic approaches lack selectivity and damage both cancerous and healthy cells. In contrast, cancer immunotherapy harnesses the host's immune system to selectively target and eradicate tumor cells, offering tremendous potential for the long-term suppression of tumor growth and preventing its recurrence. However, tumors often develop immune evasion by exploiting immune checkpoints, which regulate the immune system. Among these checkpoints, programmed death protein 1 (PD-1) and its ligand (PD-L1) have garnered significant interest because they play a key role in protecting the tumor cells from immune-mediated eradication. The approval of monoclonal antibodies (mAbs) that target PD-1/PD-L1 by the Food and Drug Administration (FDA) is a milestone in immunotherapy. Although mAbs have demonstrated remarkable success in treating skin melanomas, their efficacy against other solid tumors remains limited. There is a clear need to explore new approaches to enhance the efficacy of mAbs and find more effective checkpoint inhibitors. Metal-based drugs offer a new platform to address this challenge. This review highlights the recent progress in leveraging metal complexes as PD-1/PD-L1 inhibitors. We discussed metal-based agents used either alone or in combination with mAbs to boost the immune system. We also highlighted examples of metallodrugs encapsulated within the nanoparticles to augment the efficacy of immune checkpoint therapy. While research on metal-based complexes targeting PD-1/PD-L1 is still in its infancy, the examples presented here will serve as the basis for future discussions and efforts in this emerging field. We anticipate that ongoing research in targeting immune checkpoint blockade with innovative metal-based therapeutics will enhance the scope of treatment across a wide range of cancers.
2026, 37(4): 111076
doi: 10.1016/j.cclet.2025.111076
Abstract:
Understanding the mechanisms of virus infection is pivotal for the effective prevention and treatment of viral diseases. This review provides a comprehensive overview of the latest advancements in real-time monitoring of viral dynamics within established infection models. We begin by summarizing the recent progress in fluorescent probe and labeling techniques for real-time and in situ virus tracking. Next, we provide an in-depth analysis of the types and characteristics of virus infection models and discuss their respective advantages and limitations in virus tracking. Finally, we detail the recent progress in viral dynamics tracking across different infection models, illustrating how to use these models to monitor virus infection dynamics and discussing the meaningful biological information that can be acquired.
Understanding the mechanisms of virus infection is pivotal for the effective prevention and treatment of viral diseases. This review provides a comprehensive overview of the latest advancements in real-time monitoring of viral dynamics within established infection models. We begin by summarizing the recent progress in fluorescent probe and labeling techniques for real-time and in situ virus tracking. Next, we provide an in-depth analysis of the types and characteristics of virus infection models and discuss their respective advantages and limitations in virus tracking. Finally, we detail the recent progress in viral dynamics tracking across different infection models, illustrating how to use these models to monitor virus infection dynamics and discussing the meaningful biological information that can be acquired.
2026, 37(4): 111140
doi: 10.1016/j.cclet.2025.111140
Abstract:
Bone-related diseases resulting from accidents, illnesses, and injuries have become increasingly common in recent years. Treating these conditions poses significant challenges, including prolonged recovery times, high costs, and unpredictable outcomes, which can lead to complications such as infections and reduced muscle strength. Although autologous bone transplantation is regarded as the "gold standard" for addressing bone diseases, its application is often limited by complications at the donor site and the risk of infection. This underscores the urgent need to explore alternatives to autogenous bone transplantation. In response, a range of biomaterials for bone repair have been developed, with metal-based biomaterials emerging as effective adjuncts that enhance and optimize the repair and regeneration of bone tissue. These materials can actively influence the bone repair process through mechanisms such as inductive osteogenesis, immunomodulation, and pro-angiogenesis. This review begins by highlighting the biological effects of metal-based biomaterials, followed by a comprehensive overview of their macro- and micro-scale classifications and applications for treating various bone diseases. Finally, the review addresses future directions and challenges associated with the use of metal-based biomaterials in bone repair, aiming to propose promising strategies for the treatment of bone-related diseases.
Bone-related diseases resulting from accidents, illnesses, and injuries have become increasingly common in recent years. Treating these conditions poses significant challenges, including prolonged recovery times, high costs, and unpredictable outcomes, which can lead to complications such as infections and reduced muscle strength. Although autologous bone transplantation is regarded as the "gold standard" for addressing bone diseases, its application is often limited by complications at the donor site and the risk of infection. This underscores the urgent need to explore alternatives to autogenous bone transplantation. In response, a range of biomaterials for bone repair have been developed, with metal-based biomaterials emerging as effective adjuncts that enhance and optimize the repair and regeneration of bone tissue. These materials can actively influence the bone repair process through mechanisms such as inductive osteogenesis, immunomodulation, and pro-angiogenesis. This review begins by highlighting the biological effects of metal-based biomaterials, followed by a comprehensive overview of their macro- and micro-scale classifications and applications for treating various bone diseases. Finally, the review addresses future directions and challenges associated with the use of metal-based biomaterials in bone repair, aiming to propose promising strategies for the treatment of bone-related diseases.
2026, 37(4): 111600
doi: 10.1016/j.cclet.2025.111600
Abstract:
Iron-based nanoparticles (Fe-NPs) have wide environmental applications in various areas due to their excellent physicochemical properties, and these processes also increase their release into the water environment. However, the existing literature on environmental behavior fate (e.g., sorption and transformation) and potential ecotoxicity of Fe-NPs remains limited, which is vital for understanding the Fe-NPs environmental behavior and application as a multifunctional product. In this review, the green synthesis, characterization, and environmental application of Fe-NPs are summarized. We systematically examined the impacts of Fe-NPs physicochemical properties on its adsorption, transformation (e.g., aggregation dispersion, dissolution, oxidation), and biodegradation behavior in aqueous ecosystems. Moreover, we highlight the potential ecological toxicity of Fe-NPs to aquatic organisms. Upon exposure in water environments, Fe-NPs have potential ecological toxicity on aquatic organisms (e.g., microorganisms, plants, zooplankton, and fish). The common mechanisms of Fe-NPs ecotoxicity (e.g., bioaccumulation, oxidation stress, and DNA damage) at the cellular level are presented and the remaining unclear points on nano-toxic mechanisms (e.g., metabolic disturbance, genotoxicity) are discussed. Given the unresolved issues, the substantial gaps and the environmental risk assessment of Fe-NPs require further attention in the future. This paper will provide useful information for assessing the fate and potential ecological risks associated with Fe-NPs in aquatic environments.
Iron-based nanoparticles (Fe-NPs) have wide environmental applications in various areas due to their excellent physicochemical properties, and these processes also increase their release into the water environment. However, the existing literature on environmental behavior fate (e.g., sorption and transformation) and potential ecotoxicity of Fe-NPs remains limited, which is vital for understanding the Fe-NPs environmental behavior and application as a multifunctional product. In this review, the green synthesis, characterization, and environmental application of Fe-NPs are summarized. We systematically examined the impacts of Fe-NPs physicochemical properties on its adsorption, transformation (e.g., aggregation dispersion, dissolution, oxidation), and biodegradation behavior in aqueous ecosystems. Moreover, we highlight the potential ecological toxicity of Fe-NPs to aquatic organisms. Upon exposure in water environments, Fe-NPs have potential ecological toxicity on aquatic organisms (e.g., microorganisms, plants, zooplankton, and fish). The common mechanisms of Fe-NPs ecotoxicity (e.g., bioaccumulation, oxidation stress, and DNA damage) at the cellular level are presented and the remaining unclear points on nano-toxic mechanisms (e.g., metabolic disturbance, genotoxicity) are discussed. Given the unresolved issues, the substantial gaps and the environmental risk assessment of Fe-NPs require further attention in the future. This paper will provide useful information for assessing the fate and potential ecological risks associated with Fe-NPs in aquatic environments.
2026, 37(4): 111611
doi: 10.1016/j.cclet.2025.111611
Abstract:
Conjugated microporous polymers (CMPs) are a class of materials characterized by their rigid π-conjugated network, adjustable microporous structures, and high mechanical strength. Due to these exceptional structural features, CMPs have demonstrated outstanding potential and performance in molecular separation, energy storage, sensors, optoelectronic devices, and catalysts. It has garnered significant attention. However, despite the considerable attention and work paid to synthesizing CMP, the challenges associated with processing it in powders are frequently disregarded. Thus, future advancements must focus on developing strategies to obtain CMPs as film form and how they performed when they are integrated in devices such as batteries, LEDs, supercapacitors, sensors, and solar cells. This paper provides a comprehensive and detailed review of the most recent advances in fabrication strategies and their applications for CMP films as well as the challenges.
Conjugated microporous polymers (CMPs) are a class of materials characterized by their rigid π-conjugated network, adjustable microporous structures, and high mechanical strength. Due to these exceptional structural features, CMPs have demonstrated outstanding potential and performance in molecular separation, energy storage, sensors, optoelectronic devices, and catalysts. It has garnered significant attention. However, despite the considerable attention and work paid to synthesizing CMP, the challenges associated with processing it in powders are frequently disregarded. Thus, future advancements must focus on developing strategies to obtain CMPs as film form and how they performed when they are integrated in devices such as batteries, LEDs, supercapacitors, sensors, and solar cells. This paper provides a comprehensive and detailed review of the most recent advances in fabrication strategies and their applications for CMP films as well as the challenges.
2026, 37(4): 111632
doi: 10.1016/j.cclet.2025.111632
Abstract:
Most bioactive compounds (amino acids, sugars, peptides, proteins) and drugs are chiral. Although the enantiomers have similar physical and chemical properties, they may exhibit completely different physiological effects in terms of biological activity, toxicity, and pharmacological effects. Therefore, chiral recognition is particularly important in numerous fields. Surface-enhanced Raman scattering (SERS) spectroscopy, a promising nondestructive analytical technique with wide applications in biosensing, food safety, and environmental analysis, exhibits exceptional potential for chiral recognition. However, there remains a notable scarcity of comprehensive reviews focusing on SERS-based chiral recognition. This review introduced the development of SERS and summarized the classification of chiral enantiomers recognition by SERS spectroscopy in detail in the past 10 years, mainly including EM-dominated chiral substrates, chiral ligand-modified systems, charge transfer (CT)-based "chiral-label-free" approaches, and chiral molecularly imprinted strategies. In addition, the potential challenges and prospects in SERS spectroscopy for chiral recognition are proposed, which is expected to effectively guide future research.
Most bioactive compounds (amino acids, sugars, peptides, proteins) and drugs are chiral. Although the enantiomers have similar physical and chemical properties, they may exhibit completely different physiological effects in terms of biological activity, toxicity, and pharmacological effects. Therefore, chiral recognition is particularly important in numerous fields. Surface-enhanced Raman scattering (SERS) spectroscopy, a promising nondestructive analytical technique with wide applications in biosensing, food safety, and environmental analysis, exhibits exceptional potential for chiral recognition. However, there remains a notable scarcity of comprehensive reviews focusing on SERS-based chiral recognition. This review introduced the development of SERS and summarized the classification of chiral enantiomers recognition by SERS spectroscopy in detail in the past 10 years, mainly including EM-dominated chiral substrates, chiral ligand-modified systems, charge transfer (CT)-based "chiral-label-free" approaches, and chiral molecularly imprinted strategies. In addition, the potential challenges and prospects in SERS spectroscopy for chiral recognition are proposed, which is expected to effectively guide future research.
2026, 37(4): 111637
doi: 10.1016/j.cclet.2025.111637
Abstract:
Electrocatalysis stands as a cornerstone in the pursuit of clean energy conversion and environmental sustainability, with single-atom catalysts (SACs) emerging as a transformative paradigm for enhancing electrocatalytic efficiency. In the architectural design of SACs, supports transcend conventional roles as mere supports, actively governing catalytic performance via robust metal-support interactions (SMSI). This review comprehensively analyses the key role of support engineering in modulating SACs performance. The study begins with a systematic assessment of currently popular SACs synthesis strategies, critically comparing their advantages and limitations. Through a hierarchical analysis, it reveals the impact of various support materials, such as carbon-based materials, metal oxides, MXenes, and metal-organic frameworks (MOFs), on the catalytic performance of SACs, with emphasis on their structural characteristics, electronic properties, and interaction mechanisms with active sites. The review further explores applications in energy conversion/storage and environmental remediation, while addressing current challenges and proposing future research directions for SACs development. By providing actionable insights, this work aims to guide the design of next-generation SACs and advance sustainable electrocatalysis.
Electrocatalysis stands as a cornerstone in the pursuit of clean energy conversion and environmental sustainability, with single-atom catalysts (SACs) emerging as a transformative paradigm for enhancing electrocatalytic efficiency. In the architectural design of SACs, supports transcend conventional roles as mere supports, actively governing catalytic performance via robust metal-support interactions (SMSI). This review comprehensively analyses the key role of support engineering in modulating SACs performance. The study begins with a systematic assessment of currently popular SACs synthesis strategies, critically comparing their advantages and limitations. Through a hierarchical analysis, it reveals the impact of various support materials, such as carbon-based materials, metal oxides, MXenes, and metal-organic frameworks (MOFs), on the catalytic performance of SACs, with emphasis on their structural characteristics, electronic properties, and interaction mechanisms with active sites. The review further explores applications in energy conversion/storage and environmental remediation, while addressing current challenges and proposing future research directions for SACs development. By providing actionable insights, this work aims to guide the design of next-generation SACs and advance sustainable electrocatalysis.
2026, 37(4): 111669
doi: 10.1016/j.cclet.2025.111669
Abstract:
Sustainable and efficient solutions are essential to address increasingly critical environmental issues, particularly in the field of pollutant removal and resource recovery. The latest research has shown that pulsed electrochemistry significantly contributes to these goals by precisely altering the local reaction environment, accelerating the reaction kinetics and decreasing the overall energy requirements. However, knowledge gaps exist in dynamic evolution mechanism of electric double layer (EDL) in this technology, and challenges remain toward fully implementation of this promising technology. In this review, the fundamentals of pulsed electrochemistry and its connection to the theoretical models of EDL are comprehensively presented. The critical parameters (e.g., duty ratio, frequency and waveform) for boosting the performance of the system are systematically discussed and the typical electrochemical reactions that occur with pulsed electrochemistry are outlined. The proposed pulsed electrochemistry methodologies tailored for environmental applications are also reviewed in detail. Finally, future opportunities and challenges of this promising but fledgling field are discussed, with the expectation that this technology offers a route to transform conventional chemical industries into cleaner and more sustainable production.
Sustainable and efficient solutions are essential to address increasingly critical environmental issues, particularly in the field of pollutant removal and resource recovery. The latest research has shown that pulsed electrochemistry significantly contributes to these goals by precisely altering the local reaction environment, accelerating the reaction kinetics and decreasing the overall energy requirements. However, knowledge gaps exist in dynamic evolution mechanism of electric double layer (EDL) in this technology, and challenges remain toward fully implementation of this promising technology. In this review, the fundamentals of pulsed electrochemistry and its connection to the theoretical models of EDL are comprehensively presented. The critical parameters (e.g., duty ratio, frequency and waveform) for boosting the performance of the system are systematically discussed and the typical electrochemical reactions that occur with pulsed electrochemistry are outlined. The proposed pulsed electrochemistry methodologies tailored for environmental applications are also reviewed in detail. Finally, future opportunities and challenges of this promising but fledgling field are discussed, with the expectation that this technology offers a route to transform conventional chemical industries into cleaner and more sustainable production.
2026, 37(4): 111733
doi: 10.1016/j.cclet.2025.111733
Abstract:
Iron-based metal oxide catalysts are widely used for selective catalytic reduction (SCR) of NOx with NH3 due to their excellent catalytic performance at medium and high temperatures, high nitrogen selectivity, robust resistance to sulfur dioxide poisoning, environmental sustainability and cost effectiveness. However, several challenges including sub-optimal low-temperature catalytic activity, narrow operating temperature range, poor resistance to alkali/alkaline earth metal poisoning, as well as insufficient thermal stability and H2O/SO2 resistance always hinder the further application of iron-based metal oxide catalysts, which is in urgent need of further improvement in practical applications. This review provides a comprehensive overview of the development, applications and challenges associated with different types of iron-based metal oxide catalysts and suggests corresponding modification strategies to address the as-mentioned issues. Iron oxide catalysts can promote low-temperature catalytic performance by adjusting crystal structures and exposing specific crystal faces; however, their thermal stability and resistance to SO2/H2O and alkali metals still have substantial room for improvement. Iron-based composite metal oxide catalysts can effectively increase the resistance to SO2/H2O by coupling multiple metals and modulating adjacent electronic sites. Iron-based acidic salt catalysts greatly enhance the resistance to alkali metal poisoning by enriching the surface acid sites and providing sacrificial sites. Supported iron-based metal oxide catalysts can significantly improve both catalytic performance and resistance by modulating reaction pathways and constructing core-shell structures. This review clarifies the important direction of further research on iron-based metal oxide catalysts, and provides scientific basis and design ideas for the development and application of high-efficiency low-temperature NOx reduction catalysts.
Iron-based metal oxide catalysts are widely used for selective catalytic reduction (SCR) of NOx with NH3 due to their excellent catalytic performance at medium and high temperatures, high nitrogen selectivity, robust resistance to sulfur dioxide poisoning, environmental sustainability and cost effectiveness. However, several challenges including sub-optimal low-temperature catalytic activity, narrow operating temperature range, poor resistance to alkali/alkaline earth metal poisoning, as well as insufficient thermal stability and H2O/SO2 resistance always hinder the further application of iron-based metal oxide catalysts, which is in urgent need of further improvement in practical applications. This review provides a comprehensive overview of the development, applications and challenges associated with different types of iron-based metal oxide catalysts and suggests corresponding modification strategies to address the as-mentioned issues. Iron oxide catalysts can promote low-temperature catalytic performance by adjusting crystal structures and exposing specific crystal faces; however, their thermal stability and resistance to SO2/H2O and alkali metals still have substantial room for improvement. Iron-based composite metal oxide catalysts can effectively increase the resistance to SO2/H2O by coupling multiple metals and modulating adjacent electronic sites. Iron-based acidic salt catalysts greatly enhance the resistance to alkali metal poisoning by enriching the surface acid sites and providing sacrificial sites. Supported iron-based metal oxide catalysts can significantly improve both catalytic performance and resistance by modulating reaction pathways and constructing core-shell structures. This review clarifies the important direction of further research on iron-based metal oxide catalysts, and provides scientific basis and design ideas for the development and application of high-efficiency low-temperature NOx reduction catalysts.
2026, 37(4): 111742
doi: 10.1016/j.cclet.2025.111742
Abstract:
The Maillard reaction (non-enzymatic browning reaction) is a complex reaction between carbonyl compounds such as reducing sugars, aldehydes and ketones and compounds containing free amino groups such as amino acids, peptides and proteins. This reaction not only affects product sensory qualities, but may also generate harmful substances such as acrylamide, polycyclic aromatic hydrocarbons, and advanced glycation end-products. These substances pose various health risks to humans, including carcinogenicity, neurotoxicity and diabetes mellitus. Therefore, monitoring the Maillard reaction process and precisely controlling reaction conditions are crucial for understanding its mechanism, optimizing product quality and ensuring product safety. This review systematically summarizes recent advancements in Maillard reaction research, outlining its fundamental processes and key influencing conditions, laying a foundation for the study of the monitoring methods of Maillard reaction process. Additionally, this review takes a cross-industry perspective to explore the applications of Maillard reaction monitoring methods (spectroscopic methods, chromatography/chromatography-mass spectrometry, electrochemical methods and nuclear magnetic resonance and enzyme linked immunosorbent assay) in various fields, including food industry, tobacco processing, biopharmaceuticals, materials science and textile dyeing. Through cross-industry applications, the challenges of monitoring the Maillard reaction process are analyzed, including the diversity of reaction products, complexity of sample preparation, and real-time monitoring. Future prospects are proposed through the challenges, including the development of advanced nanomaterials and biosensors, and the integration of machine learning into predictive modeling of reaction kinetics for application in industrial processes. The review aiming to provide valuable references and guidance for industrial safety production and process condition optimization.
The Maillard reaction (non-enzymatic browning reaction) is a complex reaction between carbonyl compounds such as reducing sugars, aldehydes and ketones and compounds containing free amino groups such as amino acids, peptides and proteins. This reaction not only affects product sensory qualities, but may also generate harmful substances such as acrylamide, polycyclic aromatic hydrocarbons, and advanced glycation end-products. These substances pose various health risks to humans, including carcinogenicity, neurotoxicity and diabetes mellitus. Therefore, monitoring the Maillard reaction process and precisely controlling reaction conditions are crucial for understanding its mechanism, optimizing product quality and ensuring product safety. This review systematically summarizes recent advancements in Maillard reaction research, outlining its fundamental processes and key influencing conditions, laying a foundation for the study of the monitoring methods of Maillard reaction process. Additionally, this review takes a cross-industry perspective to explore the applications of Maillard reaction monitoring methods (spectroscopic methods, chromatography/chromatography-mass spectrometry, electrochemical methods and nuclear magnetic resonance and enzyme linked immunosorbent assay) in various fields, including food industry, tobacco processing, biopharmaceuticals, materials science and textile dyeing. Through cross-industry applications, the challenges of monitoring the Maillard reaction process are analyzed, including the diversity of reaction products, complexity of sample preparation, and real-time monitoring. Future prospects are proposed through the challenges, including the development of advanced nanomaterials and biosensors, and the integration of machine learning into predictive modeling of reaction kinetics for application in industrial processes. The review aiming to provide valuable references and guidance for industrial safety production and process condition optimization.
2026, 37(4): 111850
doi: 10.1016/j.cclet.2025.111850
Abstract:
Zinc ion hybrid capacitors (ZIHCs) are emerging electrochemical energy storage devices with the dual characteristics of high energy density and high power density. However, the mismatch of capacity and electrode kinetics between porous carbon cathodes and zinc metal anodes limits the development of ZIHCs. Lignin has high carbon content, high aromaticity, and three-dimensional functional molecular structures, which is an ideal raw material for preparing high-performance porous carbon electrode materials with high carbon yield, conductive carbon network and enriched heteroatom dopants. Currently, the high-value utilization ratio of industrial lignin is lower than 10%. In this review, the typical preparation methodologies of lignin-derived porous carbons are summarized. The latest research advances for the lignin-derived porous carbon cathodes in ZIHCs are critically focused from the perspectives of pore regulation, surface modification, and morphology design. The core points and development directions that lignin-derived porous carbon cathodes are expected to achieve an original breakthrough in the future are proposed from three levels of techniques, mechanisms, and applications. This review fills the blank region in the applications of lignin-derived porous carbons for ZIHCs, aiming to provide valuable guidance for the high-value utilization process of lignin and the industrialization process of ZIHCs.
Zinc ion hybrid capacitors (ZIHCs) are emerging electrochemical energy storage devices with the dual characteristics of high energy density and high power density. However, the mismatch of capacity and electrode kinetics between porous carbon cathodes and zinc metal anodes limits the development of ZIHCs. Lignin has high carbon content, high aromaticity, and three-dimensional functional molecular structures, which is an ideal raw material for preparing high-performance porous carbon electrode materials with high carbon yield, conductive carbon network and enriched heteroatom dopants. Currently, the high-value utilization ratio of industrial lignin is lower than 10%. In this review, the typical preparation methodologies of lignin-derived porous carbons are summarized. The latest research advances for the lignin-derived porous carbon cathodes in ZIHCs are critically focused from the perspectives of pore regulation, surface modification, and morphology design. The core points and development directions that lignin-derived porous carbon cathodes are expected to achieve an original breakthrough in the future are proposed from three levels of techniques, mechanisms, and applications. This review fills the blank region in the applications of lignin-derived porous carbons for ZIHCs, aiming to provide valuable guidance for the high-value utilization process of lignin and the industrialization process of ZIHCs.
2026, 37(4): 111892
doi: 10.1016/j.cclet.2025.111892
Abstract:
Enantioselective enamine catalysis has enriched asymmetric synthesis by enabling precise stereochemical control. While classically thermal/photochemical strategies have expanded reaction diversity, electrochemical enantiocontrol remains underexplored despite its potential for tunable redox manipulation. This review systematically evaluates electrochemical enantioselective enamine catalysis through polar/radical mediated chemical bond formation pathways, aiming to delineate current mechanistic paradigms and highlight electrochemistry's unique role on asymmetric enamine catalysis beyond thermodynamic and photochemical conditions. Future efforts including developing enhanced compatibility of chiral catalysts and intermediates with electrochemical systems, as well as exploiting transformative techniques for mechanistic elucidation could be promising to unlock more novel transformations and stereoselectivity models.
Enantioselective enamine catalysis has enriched asymmetric synthesis by enabling precise stereochemical control. While classically thermal/photochemical strategies have expanded reaction diversity, electrochemical enantiocontrol remains underexplored despite its potential for tunable redox manipulation. This review systematically evaluates electrochemical enantioselective enamine catalysis through polar/radical mediated chemical bond formation pathways, aiming to delineate current mechanistic paradigms and highlight electrochemistry's unique role on asymmetric enamine catalysis beyond thermodynamic and photochemical conditions. Future efforts including developing enhanced compatibility of chiral catalysts and intermediates with electrochemical systems, as well as exploiting transformative techniques for mechanistic elucidation could be promising to unlock more novel transformations and stereoselectivity models.
2026, 37(4): 111955
doi: 10.1016/j.cclet.2025.111955
Abstract:
Traditional cancer therapies are limited by side effects and damage to healthy tissues, while modern targeted treatments face challenges such as drug resistance and restricted applicability across cancer types. Early diagnosis also remains difficult, as many methods lack the sensitivity and specificity needed to reliably detect small, early-stage tumors. This review explores hybrid nanomaterial-based delivery systems, such as lipid–gold nanoparticle composites combined with polymeric nanocarriers, to improve the precision and efficacy of gene therapy. Advances in nanotechnology are highlighted for their ability to augment gene-editing tools including RNA interference and clustered regularly interspaced short palindromic repeats/CRISPR-associated protein 9 (CRISPR/Cas9), supported by techniques like optical tweezers, plasmonics, fluorescence imaging, and metamaterials. Nanophotonics in particular offers ultra-sensitive molecular imaging and real-time biomarker detection, underscoring its value for early cancer diagnosis. Artificial intelligence further strengthens these approaches by optimizing nanocarrier design, predicting therapeutic outcomes, and guiding personalized treatment strategies. Machine learning and deep learning platforms enable efficient analysis of complex genomic and clinical datasets, improving predictive accuracy and therapeutic customization. The review also outlines molecular mechanisms of gene therapy, from editing to expression, and addresses barriers to clinical translation, such as data integration, model validation, and regulatory considerations. Combining nanotechnology, artificial intelligence (AI), and gene-editing advances holds promise for more effective, targeted, and minimally invasive cancer treatments. These integrated strategies support earlier detection, enhance therapeutic precision, and provide a framework for translating experimental breakthroughs into clinical applications that better align with the goals of personalized medicine.
Traditional cancer therapies are limited by side effects and damage to healthy tissues, while modern targeted treatments face challenges such as drug resistance and restricted applicability across cancer types. Early diagnosis also remains difficult, as many methods lack the sensitivity and specificity needed to reliably detect small, early-stage tumors. This review explores hybrid nanomaterial-based delivery systems, such as lipid–gold nanoparticle composites combined with polymeric nanocarriers, to improve the precision and efficacy of gene therapy. Advances in nanotechnology are highlighted for their ability to augment gene-editing tools including RNA interference and clustered regularly interspaced short palindromic repeats/CRISPR-associated protein 9 (CRISPR/Cas9), supported by techniques like optical tweezers, plasmonics, fluorescence imaging, and metamaterials. Nanophotonics in particular offers ultra-sensitive molecular imaging and real-time biomarker detection, underscoring its value for early cancer diagnosis. Artificial intelligence further strengthens these approaches by optimizing nanocarrier design, predicting therapeutic outcomes, and guiding personalized treatment strategies. Machine learning and deep learning platforms enable efficient analysis of complex genomic and clinical datasets, improving predictive accuracy and therapeutic customization. The review also outlines molecular mechanisms of gene therapy, from editing to expression, and addresses barriers to clinical translation, such as data integration, model validation, and regulatory considerations. Combining nanotechnology, artificial intelligence (AI), and gene-editing advances holds promise for more effective, targeted, and minimally invasive cancer treatments. These integrated strategies support earlier detection, enhance therapeutic precision, and provide a framework for translating experimental breakthroughs into clinical applications that better align with the goals of personalized medicine.
2026, 37(4): 112036
doi: 10.1016/j.cclet.2025.112036
Abstract:
In contrast to conventional cancer treatment modalities, cancer immunotherapy has increasingly emerged as one of the most promising therapeutic approaches for cancer, owing to its capacity to elicit long-lasting immune memory and its favorable safety profile. However, the immunosuppressive tumor microenvironment (ITME) significantly hinders its progression. While tumor stromal cells play a crucial role in the formation of the ITME, they also offer several potential targets for interventions aimed at reshaping this suppressive milieu. In clinical practice, the modulating of tumor stromal cells overcomes resistance mechanisms, exhibits broader therapeutic potential, and allows for more manageable toxicity profiles. Owing to the capacity of nanodrug delivery systems (nano-DDS) to facilitate accurate targeting and integrate multiple functions, a growing number of researchers are employing nano-DDS in the immunotherapy modulated to tumor stromal cells. This review begins by elucidating the roles played by different tumor stromal cells in the formation of the ITME. Subsequently, we provide the nanodelivery strategies modulating distinct tumor stromal cells. Finally, we propose the current challenges and discuss potential future development directions in this field.
In contrast to conventional cancer treatment modalities, cancer immunotherapy has increasingly emerged as one of the most promising therapeutic approaches for cancer, owing to its capacity to elicit long-lasting immune memory and its favorable safety profile. However, the immunosuppressive tumor microenvironment (ITME) significantly hinders its progression. While tumor stromal cells play a crucial role in the formation of the ITME, they also offer several potential targets for interventions aimed at reshaping this suppressive milieu. In clinical practice, the modulating of tumor stromal cells overcomes resistance mechanisms, exhibits broader therapeutic potential, and allows for more manageable toxicity profiles. Owing to the capacity of nanodrug delivery systems (nano-DDS) to facilitate accurate targeting and integrate multiple functions, a growing number of researchers are employing nano-DDS in the immunotherapy modulated to tumor stromal cells. This review begins by elucidating the roles played by different tumor stromal cells in the formation of the ITME. Subsequently, we provide the nanodelivery strategies modulating distinct tumor stromal cells. Finally, we propose the current challenges and discuss potential future development directions in this field.
2026, 37(4): 112220
doi: 10.1016/j.cclet.2025.112220
Abstract:
Inspired by the natural synthesis of biomolecules, the artificial production of therapeutic agents within cells has emerged as a powerful and versatile approach for disease treatment. Performing artificial chemical reactions within living cells to achieve various physiological goals remains both an intriguing and highly challenging endeavor. This review summarizes recent advancements and future trends in the field of chemical reactions inside living cells, organized by different reaction mechanisms. We also provide an in-depth discussion of their chemical designs, reaction mechanisms, and functional applications. Furthermore, we explore the underlying chemical principles of these reactions and discuss strategies for these materials to enhance their therapeutic efficacy. As researchers continue to expand the repertoire of intracellular synthesis techniques, it is anticipated that these advancements will provide valuable tools for probing biological systems and developing innovative therapeutic strategies.
Inspired by the natural synthesis of biomolecules, the artificial production of therapeutic agents within cells has emerged as a powerful and versatile approach for disease treatment. Performing artificial chemical reactions within living cells to achieve various physiological goals remains both an intriguing and highly challenging endeavor. This review summarizes recent advancements and future trends in the field of chemical reactions inside living cells, organized by different reaction mechanisms. We also provide an in-depth discussion of their chemical designs, reaction mechanisms, and functional applications. Furthermore, we explore the underlying chemical principles of these reactions and discuss strategies for these materials to enhance their therapeutic efficacy. As researchers continue to expand the repertoire of intracellular synthesis techniques, it is anticipated that these advancements will provide valuable tools for probing biological systems and developing innovative therapeutic strategies.
2026, 37(4): 110733
doi: 10.1016/j.cclet.2024.110733
Abstract:
Modulating the exposed facets of metal-organic frameworks (MOFs) is an effective strategy to enhance the synergistic effects between adsorption and photocatalytic reduction of U(Ⅵ). Herein, we successfully synthesized four morphologically distinct types of NH2-MIL-125(Ti), offering insights into the impact of facet engineering on the combined adsorption and photoreduction of U(Ⅵ). An elevated exposure ratio of the {001} facet endows NH2-MIL-125(Ti) with a larger surface area, enhanced light absorption, and efficient separation of photogenerated charge carriers. Among the four photocatalysts (W, D, S and T), T with a high proportion of {001} facets, demonstrated outstanding adsorption-photocatalytic synergy, achieving over 97% of U(Ⅵ) within 20 min of visible light irradiation across a broad concentrations and pH range, without requiring a hole-trapping agent. The uranium extraction mechanism involves U(Ⅵ) coordination and chelation with active sites during adsorption, followed by reduction to U(Ⅳ) via photogenerated electrons during photocatalysis. This study highlights the use of facet engineering to enhance adsorption and photocatalytic efficiency in MOF-based photocatalysts.
Modulating the exposed facets of metal-organic frameworks (MOFs) is an effective strategy to enhance the synergistic effects between adsorption and photocatalytic reduction of U(Ⅵ). Herein, we successfully synthesized four morphologically distinct types of NH2-MIL-125(Ti), offering insights into the impact of facet engineering on the combined adsorption and photoreduction of U(Ⅵ). An elevated exposure ratio of the {001} facet endows NH2-MIL-125(Ti) with a larger surface area, enhanced light absorption, and efficient separation of photogenerated charge carriers. Among the four photocatalysts (W, D, S and T), T with a high proportion of {001} facets, demonstrated outstanding adsorption-photocatalytic synergy, achieving over 97% of U(Ⅵ) within 20 min of visible light irradiation across a broad concentrations and pH range, without requiring a hole-trapping agent. The uranium extraction mechanism involves U(Ⅵ) coordination and chelation with active sites during adsorption, followed by reduction to U(Ⅳ) via photogenerated electrons during photocatalysis. This study highlights the use of facet engineering to enhance adsorption and photocatalytic efficiency in MOF-based photocatalysts.
2026, 37(4): 110749
doi: 10.1016/j.cclet.2024.110749
Abstract:
Water electrolysis for practical applications faces challenges such as slow kinetics of catalysts in oxygen evolution reaction (OER). These can be effectively improved by facilitating the migration of oxygen intermediates at the material's interface. In this work, we employed carbon dots to modify a heterophase Ir-based oxide catalyst (h-IrO2@CDs) to improve their acidic OER performance. Experimental and theoretical studies reveal that CDs enhances oxygen intermediate migration between rutile and 1T phases, enabling a synergistic oxidation pathway. The small amount addition of CDs reduces energy barriers in the rate-determining step and mitigates excessive oxidation, which significantly boost catalytic activity and stability of IrO2@CDs. The optimal h-IrO2@CDs-3 catalyst achieves a low overpotential (161 mV) for 10 mA/cm2 OER current and remains stable for > 762 h at 10 mA/cm2. The low cost and easy synthesis make CDs highly promising for enhancing overall performance in catalytic fields.
Water electrolysis for practical applications faces challenges such as slow kinetics of catalysts in oxygen evolution reaction (OER). These can be effectively improved by facilitating the migration of oxygen intermediates at the material's interface. In this work, we employed carbon dots to modify a heterophase Ir-based oxide catalyst (h-IrO2@CDs) to improve their acidic OER performance. Experimental and theoretical studies reveal that CDs enhances oxygen intermediate migration between rutile and 1T phases, enabling a synergistic oxidation pathway. The small amount addition of CDs reduces energy barriers in the rate-determining step and mitigates excessive oxidation, which significantly boost catalytic activity and stability of IrO2@CDs. The optimal h-IrO2@CDs-3 catalyst achieves a low overpotential (161 mV) for 10 mA/cm2 OER current and remains stable for > 762 h at 10 mA/cm2. The low cost and easy synthesis make CDs highly promising for enhancing overall performance in catalytic fields.
2026, 37(4): 110750
doi: 10.1016/j.cclet.2024.110750
Abstract:
Proton-conducting materials are essential for energy and electronic technologies. Polyoxometalates (POMs), as molecularly well-defined metal oxide nanoclusters with high proton conductivity, are promising candidates for such applications. However, their intrinsic crystalline brittleness poses significant challenges for practical device processing. In this work, we present a strategy to incorporate POM nanoclusters into supramolecular ionic networks (SINs). By using synergistic electrostatic and hydrogen bonding interactions, we uniformly disperse POM nanoclusters into zwitterionic liquids, forming an ionic network structure. The resulting POM-based SIN electrolytes exhibit semi-solid flexibility and high proton conductivity of 2.0 × 10-3 S/cm. Notably, these electrolytes demonstrate strong adhesion with activated carbon electrodes, resulting in flexible supercapacitors with a stable electrolyte-electrode interface that retains 90% capacitance after 14,000 charge-discharge cycles and 10,000 bending cycles. This study provides a promising approach for developing nanocluster-based soft electrolyte materials for flexible devices.
Proton-conducting materials are essential for energy and electronic technologies. Polyoxometalates (POMs), as molecularly well-defined metal oxide nanoclusters with high proton conductivity, are promising candidates for such applications. However, their intrinsic crystalline brittleness poses significant challenges for practical device processing. In this work, we present a strategy to incorporate POM nanoclusters into supramolecular ionic networks (SINs). By using synergistic electrostatic and hydrogen bonding interactions, we uniformly disperse POM nanoclusters into zwitterionic liquids, forming an ionic network structure. The resulting POM-based SIN electrolytes exhibit semi-solid flexibility and high proton conductivity of 2.0 × 10-3 S/cm. Notably, these electrolytes demonstrate strong adhesion with activated carbon electrodes, resulting in flexible supercapacitors with a stable electrolyte-electrode interface that retains 90% capacitance after 14,000 charge-discharge cycles and 10,000 bending cycles. This study provides a promising approach for developing nanocluster-based soft electrolyte materials for flexible devices.
2026, 37(4): 110751
doi: 10.1016/j.cclet.2024.110751
Abstract:
Lithium-ion batteries (LIBs) are essential energy storage devices widely used in portable electronics, transportation, and various other applications. However, current anode materials, with their low intercalation potentials and poor rate performance, struggle to balance energy density, power density, and safety, particularly under extreme conditions. In this work, we report a self-regulating micro-channel network that forms a three-dimensional (3D) composite electrode architecture without binders and conductive additives, offering a promising anode solution for fast-charging LIBs. Benefiting from the robust 3D architecture with abundant Li+ active sites and superior electronic conductivity, the niobium tungsten oxide@carbon nanotube (NWO/CNT) composite electrode demonstrates a high reversible capacity (246.6 mAh/g at 0.2 C), excellent rate capability (117.1 mAh/g at 60 C), and long-term durability (73.0% capacity retention after 10,000 cycles). Additionally, a thick electrode with high mass loading (10 mg/cm2) shows remarkable high-rate performance, retaining 51.7% capacity at 20 C. Notably, when paired with LiFePO4 (LFP) cathodes, the NWO@CNT//LFP@CNT full batteries exhibit impressive high-power capability (2.8 kW/kg), high energy density (394.2 Wh/kg), and exceptional cycle stability (82% capacity retention after 6000 cycles). Most importantly, this composite electrode architecture also enables the fabrication of a planar, miniaturized, all-solid-state lithium-ion battery with fast-charging capabilities.
Lithium-ion batteries (LIBs) are essential energy storage devices widely used in portable electronics, transportation, and various other applications. However, current anode materials, with their low intercalation potentials and poor rate performance, struggle to balance energy density, power density, and safety, particularly under extreme conditions. In this work, we report a self-regulating micro-channel network that forms a three-dimensional (3D) composite electrode architecture without binders and conductive additives, offering a promising anode solution for fast-charging LIBs. Benefiting from the robust 3D architecture with abundant Li+ active sites and superior electronic conductivity, the niobium tungsten oxide@carbon nanotube (NWO/CNT) composite electrode demonstrates a high reversible capacity (246.6 mAh/g at 0.2 C), excellent rate capability (117.1 mAh/g at 60 C), and long-term durability (73.0% capacity retention after 10,000 cycles). Additionally, a thick electrode with high mass loading (10 mg/cm2) shows remarkable high-rate performance, retaining 51.7% capacity at 20 C. Notably, when paired with LiFePO4 (LFP) cathodes, the NWO@CNT//LFP@CNT full batteries exhibit impressive high-power capability (2.8 kW/kg), high energy density (394.2 Wh/kg), and exceptional cycle stability (82% capacity retention after 6000 cycles). Most importantly, this composite electrode architecture also enables the fabrication of a planar, miniaturized, all-solid-state lithium-ion battery with fast-charging capabilities.
2026, 37(4): 110754
doi: 10.1016/j.cclet.2024.110754
Abstract:
Ruthenium, possessing a comparable metal-hydrogen bond energy to Pt, has emerged as a promising electrocatalyst for the hydrogen oxidation reaction (HOR), but its practical applications are hindered by susceptibility to deactivation or dissolution under operating conditions of fuel cells. Herein, graphene-encapsulated Ru nanoparticles (Ru@NG) was employed as the HOR catalyst for high-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs). The graphene shells on the Ru can block effectively the surface adsorption of phosphoric acid in electrolyte and CO in anode fuel, but does not affect H2 free access to Ru sites, thus increase the activity expression and stability of catalysts under the high temperature, strong acid, and oxidation conditions of the HT-PEMFCs. With Ru@NG as the anode catalyst, the fuel cell delivers a peak power density of 760 mW/cm2 with pure H2, and additionally, it shows better tolerance to CO that the performance is 1.5 times that of the Pt/C catalysts with H2 fuel containing 1% CO. This work provides an alternative strategy to design the electrocatalysts for HT-PEMFCs.
Ruthenium, possessing a comparable metal-hydrogen bond energy to Pt, has emerged as a promising electrocatalyst for the hydrogen oxidation reaction (HOR), but its practical applications are hindered by susceptibility to deactivation or dissolution under operating conditions of fuel cells. Herein, graphene-encapsulated Ru nanoparticles (Ru@NG) was employed as the HOR catalyst for high-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs). The graphene shells on the Ru can block effectively the surface adsorption of phosphoric acid in electrolyte and CO in anode fuel, but does not affect H2 free access to Ru sites, thus increase the activity expression and stability of catalysts under the high temperature, strong acid, and oxidation conditions of the HT-PEMFCs. With Ru@NG as the anode catalyst, the fuel cell delivers a peak power density of 760 mW/cm2 with pure H2, and additionally, it shows better tolerance to CO that the performance is 1.5 times that of the Pt/C catalysts with H2 fuel containing 1% CO. This work provides an alternative strategy to design the electrocatalysts for HT-PEMFCs.
2026, 37(4): 110755
doi: 10.1016/j.cclet.2024.110755
Abstract:
Ferroelastics have attracted considerable interest because of their promising uses in areas such as energy conversion, sensing technologies, and beyond. However, exploring ferroelastics with high-temperature dielectric switching and photoluminescence remains a challenge. Here, we have synthesized two ferroelastics (DMTP)PbBr3 (DMTP = N,N-dimethyl-1,2,3,6-tetrahydropyridine) and (DMTP)PbI3 under the guidance of halogen substitution strategy. (DMTP)PbI3 experiences the dielectric switching at 371 K, and upon halogen substitution, the strengthened intermolecular interactions lead to (DMTP)PbBr3 undergoing a similar switching at around 390 K. Additionally, two compounds both emit orange light under ultraviolet illumination. (DMTP)PbI3 has the photoluminescence quantum yield of 2.68%, while (DMTP)PbBr3, due to the increased distortion of the inorganic part after halogen substitution, achieves the higher quantum yield of 12%. This work offers meaningful perspectives on exploring the search for ferroelectrics with photoluminescence and high-temperature dielectric switching, and also demonstrates the rationality of the halogen substitution strategy.
Ferroelastics have attracted considerable interest because of their promising uses in areas such as energy conversion, sensing technologies, and beyond. However, exploring ferroelastics with high-temperature dielectric switching and photoluminescence remains a challenge. Here, we have synthesized two ferroelastics (DMTP)PbBr3 (DMTP = N,N-dimethyl-1,2,3,6-tetrahydropyridine) and (DMTP)PbI3 under the guidance of halogen substitution strategy. (DMTP)PbI3 experiences the dielectric switching at 371 K, and upon halogen substitution, the strengthened intermolecular interactions lead to (DMTP)PbBr3 undergoing a similar switching at around 390 K. Additionally, two compounds both emit orange light under ultraviolet illumination. (DMTP)PbI3 has the photoluminescence quantum yield of 2.68%, while (DMTP)PbBr3, due to the increased distortion of the inorganic part after halogen substitution, achieves the higher quantum yield of 12%. This work offers meaningful perspectives on exploring the search for ferroelectrics with photoluminescence and high-temperature dielectric switching, and also demonstrates the rationality of the halogen substitution strategy.
2026, 37(4): 110792
doi: 10.1016/j.cclet.2024.110792
Abstract:
The application of commercial hard carbon (HC) materials in sodium-ion batteries (SIBs) is limited by their inferior rate capability (<5.0 A/g) and low tap density (<1.0 g/cm3). Alloying-type bismuth (Bi) offers a high theoretical volumetric capacity of 3800 mAh/cm3 and superb rate capability but suffers from large volume expansion (~244%) and undesirable structural pulverization. Herein, a hectogram-scale Bi-inlaid carbon skeleton (GC-Bi) composite was synthesized through a facile precipitation-carbonization method using low-cost industrial-grade chemical reagents. The as-prepared GC-Bi composite features a unique particle-nested-bulk architecture, achieving a high tap-density of 3.33 g/cm3, which is approximately 4.16 times greater than that of commercial HC. Besides, the carbon sheath enhances the electronic conductivity and accommodates the substantial volume swelling of the embedded Bi particles, contributing to the formation of a thin and stable solid electrolyte interface on the electrode. Consequently, the GC-Bi anode achieves a high volumetric capacity (1123 mAh/cm3), impressive rate capability (207.8 mAh/g at 80 A/g), together with long cyclability retaining 96.5% of its capacity after 5000 cycles in a Na//GC-Bi half-cell and 78% after 800 cycles in a GC-Bi//Na3V2(PO4)3 full-cell.
The application of commercial hard carbon (HC) materials in sodium-ion batteries (SIBs) is limited by their inferior rate capability (<5.0 A/g) and low tap density (<1.0 g/cm3). Alloying-type bismuth (Bi) offers a high theoretical volumetric capacity of 3800 mAh/cm3 and superb rate capability but suffers from large volume expansion (~244%) and undesirable structural pulverization. Herein, a hectogram-scale Bi-inlaid carbon skeleton (GC-Bi) composite was synthesized through a facile precipitation-carbonization method using low-cost industrial-grade chemical reagents. The as-prepared GC-Bi composite features a unique particle-nested-bulk architecture, achieving a high tap-density of 3.33 g/cm3, which is approximately 4.16 times greater than that of commercial HC. Besides, the carbon sheath enhances the electronic conductivity and accommodates the substantial volume swelling of the embedded Bi particles, contributing to the formation of a thin and stable solid electrolyte interface on the electrode. Consequently, the GC-Bi anode achieves a high volumetric capacity (1123 mAh/cm3), impressive rate capability (207.8 mAh/g at 80 A/g), together with long cyclability retaining 96.5% of its capacity after 5000 cycles in a Na//GC-Bi half-cell and 78% after 800 cycles in a GC-Bi//Na3V2(PO4)3 full-cell.
2026, 37(4): 110824
doi: 10.1016/j.cclet.2025.110824
Abstract:
Reversible modulation of the transmittance in electrochromic devices (ECDs) holds tremendous potential for energy-saving windows. The choice of electrolyte significantly influences the optical modulation, coloring response speed, coloring efficiency, and cycling stability of electrochromic devices. Moreover, traditional electrolytes are prone to instability under extreme temperature conditions, leading to device failure and severely limiting the widespread application of smart electrochromic windows. This study introduces LiCl water-in-salt electrolyte (WiSE) into tungsten oxide-based ECDs. LiCl WiSE exhibits wide-temperature tolerance and excellent ion conductivity. Therefore, the constructed tungsten oxide ECD demonstrates large optical modulation (76.2%@700 nm), fast response time (tc = 2.0 s, tb = 1.8 s), and high cycling stability (95.8% retention after 1000 cycles). Especially, it operates efficiently over a wide temperature range of -30~80 ℃. This research provides a new approach for electrolyte selection in the fabrication of high-performance, wide-temperature-tolerant ECDs.
Reversible modulation of the transmittance in electrochromic devices (ECDs) holds tremendous potential for energy-saving windows. The choice of electrolyte significantly influences the optical modulation, coloring response speed, coloring efficiency, and cycling stability of electrochromic devices. Moreover, traditional electrolytes are prone to instability under extreme temperature conditions, leading to device failure and severely limiting the widespread application of smart electrochromic windows. This study introduces LiCl water-in-salt electrolyte (WiSE) into tungsten oxide-based ECDs. LiCl WiSE exhibits wide-temperature tolerance and excellent ion conductivity. Therefore, the constructed tungsten oxide ECD demonstrates large optical modulation (76.2%@700 nm), fast response time (tc = 2.0 s, tb = 1.8 s), and high cycling stability (95.8% retention after 1000 cycles). Especially, it operates efficiently over a wide temperature range of -30~80 ℃. This research provides a new approach for electrolyte selection in the fabrication of high-performance, wide-temperature-tolerant ECDs.
2026, 37(4): 110825
doi: 10.1016/j.cclet.2025.110825
Abstract:
Birefringent crystals have gained increasing attention for versatile optical devices due to their inherent ability to modulate light polarization. However, the rational design of structures that exhibit high birefringence and deep-ultraviolet (DUV) transparency remains a formidable challenge. Here, a novel zinc borate birefringent crystal, Na2ZnB6O11 (NZBO), was identified by strategically assembling the π-conjugated [B3O7] functional units using the unprecedented antiparallel triangles formed by [ZnO3] motifs. Remarkably, through a tailored motif approach and optimized arrangement, NZBO achieves the largest birefringence (0.094) in the visible wavelength range among the borate-based crystals containing [B3O7] units, exceeding that of commercially available birefringent crystal MgF2 by approximately 8 times (0.012@532 nm). Furthermore, NZBO exhibits a notably short DUV absorption cutoff edge below 190 nm along with a wide band gap of 6.04 eV attributed to the elimination of dangling bonds. The origin of the optical anisotropy attributes of NZBO was elucidated through a combination of theoretical calculations and structural analyses. These findings highlight the good potential of NZBO in the manipulation of polarized light and offer valuable insights for tailoring new birefringent materials in the short-wave UV transparency region.
Birefringent crystals have gained increasing attention for versatile optical devices due to their inherent ability to modulate light polarization. However, the rational design of structures that exhibit high birefringence and deep-ultraviolet (DUV) transparency remains a formidable challenge. Here, a novel zinc borate birefringent crystal, Na2ZnB6O11 (NZBO), was identified by strategically assembling the π-conjugated [B3O7] functional units using the unprecedented antiparallel triangles formed by [ZnO3] motifs. Remarkably, through a tailored motif approach and optimized arrangement, NZBO achieves the largest birefringence (0.094) in the visible wavelength range among the borate-based crystals containing [B3O7] units, exceeding that of commercially available birefringent crystal MgF2 by approximately 8 times (0.012@532 nm). Furthermore, NZBO exhibits a notably short DUV absorption cutoff edge below 190 nm along with a wide band gap of 6.04 eV attributed to the elimination of dangling bonds. The origin of the optical anisotropy attributes of NZBO was elucidated through a combination of theoretical calculations and structural analyses. These findings highlight the good potential of NZBO in the manipulation of polarized light and offer valuable insights for tailoring new birefringent materials in the short-wave UV transparency region.
2026, 37(4): 110826
doi: 10.1016/j.cclet.2025.110826
Abstract:
Ferroelectric plastic crystals have garnered significant attention in recent years due to their unique phase-transition behaviors and potential nonlinear optical properties. Nevertheless, most existing examples encounter challenges, such as inadequate transparency and diminished nonlinear optical signal, which constrain their broader applicability. In this study, we present a new ferroelectric plastic crystal, 1-azanorbornanium tetrachlorogallate, which crystallizes in the polar space group Pmc21 at room temperature and undergoes plastic phase transition at above 413 K. This phase transition endows this compound with nonlinear optical performance at polar room-temperature phase, while allowing highly-dynamic molecular rotation to provide excellent mechanical flexibility at high-temperature phase. Through hot-pressing the powder sample, a pressed tablet with an increased density that is 99.4% of crystallographic density (1.70 g/cm3) was obtained. Benefiting from the elimination of crystal grains, such a high-density tablet has significant improvements in light transmittance and second harmonic generation (SHG). Its SHG is increased by approximately 20 times and 6 times those of the loose powder form and referenced KH2PO4, respectively. This work demonstrated the potential of hot-pressing method on enhancing nonlinear optical performance of polar plastic crystals.
Ferroelectric plastic crystals have garnered significant attention in recent years due to their unique phase-transition behaviors and potential nonlinear optical properties. Nevertheless, most existing examples encounter challenges, such as inadequate transparency and diminished nonlinear optical signal, which constrain their broader applicability. In this study, we present a new ferroelectric plastic crystal, 1-azanorbornanium tetrachlorogallate, which crystallizes in the polar space group Pmc21 at room temperature and undergoes plastic phase transition at above 413 K. This phase transition endows this compound with nonlinear optical performance at polar room-temperature phase, while allowing highly-dynamic molecular rotation to provide excellent mechanical flexibility at high-temperature phase. Through hot-pressing the powder sample, a pressed tablet with an increased density that is 99.4% of crystallographic density (1.70 g/cm3) was obtained. Benefiting from the elimination of crystal grains, such a high-density tablet has significant improvements in light transmittance and second harmonic generation (SHG). Its SHG is increased by approximately 20 times and 6 times those of the loose powder form and referenced KH2PO4, respectively. This work demonstrated the potential of hot-pressing method on enhancing nonlinear optical performance of polar plastic crystals.
2026, 37(4): 111047
doi: 10.1016/j.cclet.2025.111047
Abstract:
In the process of tumor treatment, chemotherapy drugs have been widely used in clinical practice due to their broad-spectrum and significant therapeutic effects. However, the serious side effects caused by off-target effects also limit the actual efficacy of such drugs in clinical. Here, we developed a series of small molecule-drug conjugates (SMDCs) with carbonic anhydrase IX (CAIX)-targeted unit, which can deliver chemotherapy drugs to CAIX-positive cancer cells and release them in the tumor microenvironment. These SMDCs can quickly captured by the highly expressed CAIX on the tumor membrane, forming a high local concentration difference that allows SMDCs to enter the tumor cells faster. The optimized SMDC (CAIXi-R-HCPT) with ROS-sensitive linker showed higher cytotoxicity than Irinotecan. In MDA-MB-231 solid tumor-bearing mice, CAIXi-R-HCPT showed higher tumor/normal tissue (T/N) ratio than the corresponding SMDC and Irinotecan control and it also exhibited in vivo anti-tumor activity comparable to HCPT at the same dosage, and there was no significant weight loss. These findings emphasize the potential of CAIXi-R-HCPT as a promising anti-cancer SMDC that exhibits targeted delivery, tumor-specific release, and strong anti-tumor effects.
In the process of tumor treatment, chemotherapy drugs have been widely used in clinical practice due to their broad-spectrum and significant therapeutic effects. However, the serious side effects caused by off-target effects also limit the actual efficacy of such drugs in clinical. Here, we developed a series of small molecule-drug conjugates (SMDCs) with carbonic anhydrase IX (CAIX)-targeted unit, which can deliver chemotherapy drugs to CAIX-positive cancer cells and release them in the tumor microenvironment. These SMDCs can quickly captured by the highly expressed CAIX on the tumor membrane, forming a high local concentration difference that allows SMDCs to enter the tumor cells faster. The optimized SMDC (CAIXi-R-HCPT) with ROS-sensitive linker showed higher cytotoxicity than Irinotecan. In MDA-MB-231 solid tumor-bearing mice, CAIXi-R-HCPT showed higher tumor/normal tissue (T/N) ratio than the corresponding SMDC and Irinotecan control and it also exhibited in vivo anti-tumor activity comparable to HCPT at the same dosage, and there was no significant weight loss. These findings emphasize the potential of CAIXi-R-HCPT as a promising anti-cancer SMDC that exhibits targeted delivery, tumor-specific release, and strong anti-tumor effects.
2026, 37(4): 111049
doi: 10.1016/j.cclet.2025.111049
Abstract:
Heterodimerization of receptor tyrosine kinases (RTKs) plays unique roles in cell signaling and functions. However, engineering heterodimerization of multiple receptors remains largely unexplored. Herein, we developed an aptamer-based DNA Nano-windmill (TA3) to regulate heterodimerization of three different RTK families, simultaneously activating fibroblast growth factor receptor 1 (FGFR1), hepatocyte growth factor receptor (Met) and epidermal growth factor receptor (EGFR) signaling. It is the first DNA Nano-windmill that activates heterodimerization of FGFR1, Met and EGFR, leading to the down-stream signals transduction, such as the phosphorylation of protein kinase B (Akt) and extracellular regulated protein kinases (Erk), inducing the cell migration and proliferation. We further designed transformable DNA Nano-windmill (TMA) that can convert DNA Nano-windmill into DNA Nano-kite using complementary strands or small molecules to reduce the activation of specific receptor. We believe that the DNA Nano-windmill for heterodimerization of different RTK families have potential applications in biomedicine fields.
Heterodimerization of receptor tyrosine kinases (RTKs) plays unique roles in cell signaling and functions. However, engineering heterodimerization of multiple receptors remains largely unexplored. Herein, we developed an aptamer-based DNA Nano-windmill (TA3) to regulate heterodimerization of three different RTK families, simultaneously activating fibroblast growth factor receptor 1 (FGFR1), hepatocyte growth factor receptor (Met) and epidermal growth factor receptor (EGFR) signaling. It is the first DNA Nano-windmill that activates heterodimerization of FGFR1, Met and EGFR, leading to the down-stream signals transduction, such as the phosphorylation of protein kinase B (Akt) and extracellular regulated protein kinases (Erk), inducing the cell migration and proliferation. We further designed transformable DNA Nano-windmill (TMA) that can convert DNA Nano-windmill into DNA Nano-kite using complementary strands or small molecules to reduce the activation of specific receptor. We believe that the DNA Nano-windmill for heterodimerization of different RTK families have potential applications in biomedicine fields.
2026, 37(4): 111086
doi: 10.1016/j.cclet.2025.111086
Abstract:
Bacitracin has been extensively studied for its antibacterial application due to its excellent anti-Gram-positive bacterial properties. However, its application of conventional bacitracin has been limited because of its limited antibacterial activity against Gram-negative bacteria, especially negative bacilli. In this study, we designed and synthesized bacitracin-zinc nanodrugs (BPNDs) through zinc coordination self-assembly of bacitracin, which exhibit potent antibacterial effects not only against Gram-positive bacterial Staphylococcus aureus but also against Escherichia coli, a typical Gram-negative bacillus. The morphological and antimicrobial properties of the self-assembled BPNDs with different molar ratios of bacitracin to zinc ions were investigated. The bacterial biofilm experiments confirmed the biofilm scavenging effect of BPNDs, further expanding the application of this antimicrobial agent. In-depth cell viability experiments indicated that this antimicrobial activity might be related to the penetration of BPNDs into bacterial cell membranes. This study reveals that the zinc-coordinated peptide self-assembly strategy expands the antibacterial spectrum of conventional bacitracin, making it a potential candidate for novel antimicrobial drugs to address the bacterial resistance dilemma and provide stable alternatives for a wide range of biomedical and related industries.
Bacitracin has been extensively studied for its antibacterial application due to its excellent anti-Gram-positive bacterial properties. However, its application of conventional bacitracin has been limited because of its limited antibacterial activity against Gram-negative bacteria, especially negative bacilli. In this study, we designed and synthesized bacitracin-zinc nanodrugs (BPNDs) through zinc coordination self-assembly of bacitracin, which exhibit potent antibacterial effects not only against Gram-positive bacterial Staphylococcus aureus but also against Escherichia coli, a typical Gram-negative bacillus. The morphological and antimicrobial properties of the self-assembled BPNDs with different molar ratios of bacitracin to zinc ions were investigated. The bacterial biofilm experiments confirmed the biofilm scavenging effect of BPNDs, further expanding the application of this antimicrobial agent. In-depth cell viability experiments indicated that this antimicrobial activity might be related to the penetration of BPNDs into bacterial cell membranes. This study reveals that the zinc-coordinated peptide self-assembly strategy expands the antibacterial spectrum of conventional bacitracin, making it a potential candidate for novel antimicrobial drugs to address the bacterial resistance dilemma and provide stable alternatives for a wide range of biomedical and related industries.
2026, 37(4): 111119
doi: 10.1016/j.cclet.2025.111119
Abstract:
The performance of photosensitizers determines the effect of photodynamic therapy (PDT). At present, most photosensitizers are developed from fluorescent dyes, but it is difficult to possess both the good photophysical properties and photosensitive efficiency. In this work, an efficient strategy was developed to construct a cyanine-based near infrared (NIR) photosensitizer, 2LBCy5.5, with an enlarged and twisted D-π-A-π-D structure by connecting two classical Cy5.5 dyes smartly with a dual-cationic benzo[1,2-b:4,5-b']dipyrrole group. The 2LBCy5.5 exhibited a maximum absorption at 802 nm with a great molar extinction coefficient of 4.2 × 105 L mol−1 cm−1, compared with its parent Cy5.5 (692 nm with a molar extinction coefficient of 2.5 × 105 L mol−1 cm−1). Furthermore, 2LBCy5.5 exhibited narrow energy gap of singlet-triplet (ΔES-T) accelerated the intersystem crossing process (1.21 ns−1) with a high triplet-excited-state quantum yield (26.1%) under 808 nm excitation, greatly contributing to reactive oxygen species (ROS) generation in type-Ⅰ PDT. The excellent anti-tumor ability of 2LBCy5.5 was realized both under normoxic and hypoxic conditions. This study provides an effective and powerful approach for designing cyanine photosensitizers with strong capabilities in both photophysical properties (e.g., NIR light-harvesting) and highly antitumor efficiency.
The performance of photosensitizers determines the effect of photodynamic therapy (PDT). At present, most photosensitizers are developed from fluorescent dyes, but it is difficult to possess both the good photophysical properties and photosensitive efficiency. In this work, an efficient strategy was developed to construct a cyanine-based near infrared (NIR) photosensitizer, 2LBCy5.5, with an enlarged and twisted D-π-A-π-D structure by connecting two classical Cy5.5 dyes smartly with a dual-cationic benzo[1,2-b:4,5-b']dipyrrole group. The 2LBCy5.5 exhibited a maximum absorption at 802 nm with a great molar extinction coefficient of 4.2 × 105 L mol−1 cm−1, compared with its parent Cy5.5 (692 nm with a molar extinction coefficient of 2.5 × 105 L mol−1 cm−1). Furthermore, 2LBCy5.5 exhibited narrow energy gap of singlet-triplet (ΔES-T) accelerated the intersystem crossing process (1.21 ns−1) with a high triplet-excited-state quantum yield (26.1%) under 808 nm excitation, greatly contributing to reactive oxygen species (ROS) generation in type-Ⅰ PDT. The excellent anti-tumor ability of 2LBCy5.5 was realized both under normoxic and hypoxic conditions. This study provides an effective and powerful approach for designing cyanine photosensitizers with strong capabilities in both photophysical properties (e.g., NIR light-harvesting) and highly antitumor efficiency.
2026, 37(4): 111139
doi: 10.1016/j.cclet.2025.111139
Abstract:
The photopharmacology incorporated with molecular photoswitches offers a promising solution to fundamentally address the problem of bacterial resistance, simultaneously realizes the spatiotemporal precision treatment through remote light control. However, most of reported photoswitchable drugs are limited by the need of ultraviolet (UV) light, which is often damaging and not suitable for tissue penetration. Therefore, the development of photopharmacological agents triggered by visible light, especially near-infrared (NIR) light is highly desirable for future photoswitchable antibiotics. Herein, a novel photopharmacological antibacterial agent DTE-FQ was designed and synthesized by the incorporation of dithienylethene (DTE) molecular photoswitch and fluoroquinolones (FQ) antimicrobial drug norfloxacin bridged by pyridinium group and flexible butyl chain. As expected, as-prepared DTE-FQ presents efficient photoswitching behavior in various solutions upon alternating irradiation with blue light (460–470 nm) and NIR light (730–740 nm). Simultaneously, it shows significant and reversible configurational transition by the synergistic effect of DTE photoswitch and flexible butyl chain. Most remarkably, DTE-FQ reveals an at least 4-fold difference in activity against Escherichia coli (E. coli) for ring-open and ring-closed isomers, and a distinct change in bacterial growth is observed by in situ irradiation with NIR light in the presence of E. coli. These results are further confirmed by the molecular docking to DNA gyrase. The chain-like configuration of DTE-FQ treated with NIR light, inserted between the double-stranded DNA restraining the replication of DNA. Whereas the coiled configuration obtained by blue light irradiation, remained in the vicinity of the double-stranded DNA showing weak antibacterial activity. As far as we know, it represents the first example of blue-/NIR light-triggered photopharmacological antibacterial agent based on DTE switch so far, indicating its potential for in vivo photopharmacological applications.
The photopharmacology incorporated with molecular photoswitches offers a promising solution to fundamentally address the problem of bacterial resistance, simultaneously realizes the spatiotemporal precision treatment through remote light control. However, most of reported photoswitchable drugs are limited by the need of ultraviolet (UV) light, which is often damaging and not suitable for tissue penetration. Therefore, the development of photopharmacological agents triggered by visible light, especially near-infrared (NIR) light is highly desirable for future photoswitchable antibiotics. Herein, a novel photopharmacological antibacterial agent DTE-FQ was designed and synthesized by the incorporation of dithienylethene (DTE) molecular photoswitch and fluoroquinolones (FQ) antimicrobial drug norfloxacin bridged by pyridinium group and flexible butyl chain. As expected, as-prepared DTE-FQ presents efficient photoswitching behavior in various solutions upon alternating irradiation with blue light (460–470 nm) and NIR light (730–740 nm). Simultaneously, it shows significant and reversible configurational transition by the synergistic effect of DTE photoswitch and flexible butyl chain. Most remarkably, DTE-FQ reveals an at least 4-fold difference in activity against Escherichia coli (E. coli) for ring-open and ring-closed isomers, and a distinct change in bacterial growth is observed by in situ irradiation with NIR light in the presence of E. coli. These results are further confirmed by the molecular docking to DNA gyrase. The chain-like configuration of DTE-FQ treated with NIR light, inserted between the double-stranded DNA restraining the replication of DNA. Whereas the coiled configuration obtained by blue light irradiation, remained in the vicinity of the double-stranded DNA showing weak antibacterial activity. As far as we know, it represents the first example of blue-/NIR light-triggered photopharmacological antibacterial agent based on DTE switch so far, indicating its potential for in vivo photopharmacological applications.
2026, 37(4): 111141
doi: 10.1016/j.cclet.2025.111141
Abstract:
In this work, the spin-orbit charge transfer intersystem crossing (SOCT-ISC) mechanism is introduced into the near-infrared and highly photon-capturing heptamethine cyanine (Cy7) class to construct photosensitizer (PS) for photodynamic therapy (PDT) of tumor. The target PS AN–Cy7 shows an obviously improved singlet oxygen (1O2) quantum yield than the Food and Drug Administration (FDA)-approved indocyanine green (ICG) under 750 nm low-power photoirradiation (30 mW/cm2) while retaining strong fluorescence at ~805 nm. Importantly, the PS forms a 2:1 dye-human serum albumin (HSA) nanocomplex, ensuring its strong accumulation and retention at tumor site (up to five days) post intravenous injection. After a single PDT treatment, the nanocomplex almost completely ablates primary tumor while triggering an antitumor immune response to suppress the growth of distant tumors. Overall, the nanocomplex overcomes many shortcomings of clinically used PSs, thus being promising for future clinical translation.
In this work, the spin-orbit charge transfer intersystem crossing (SOCT-ISC) mechanism is introduced into the near-infrared and highly photon-capturing heptamethine cyanine (Cy7) class to construct photosensitizer (PS) for photodynamic therapy (PDT) of tumor. The target PS AN–Cy7 shows an obviously improved singlet oxygen (1O2) quantum yield than the Food and Drug Administration (FDA)-approved indocyanine green (ICG) under 750 nm low-power photoirradiation (30 mW/cm2) while retaining strong fluorescence at ~805 nm. Importantly, the PS forms a 2:1 dye-human serum albumin (HSA) nanocomplex, ensuring its strong accumulation and retention at tumor site (up to five days) post intravenous injection. After a single PDT treatment, the nanocomplex almost completely ablates primary tumor while triggering an antitumor immune response to suppress the growth of distant tumors. Overall, the nanocomplex overcomes many shortcomings of clinically used PSs, thus being promising for future clinical translation.
2026, 37(4): 111143
doi: 10.1016/j.cclet.2025.111143
Abstract:
Sirtuin 2 (SIRT2) is one of the key members of sirtuins family that plays important role in regulating many physiological processes. Recent evidences have revealed that SIRT2 is associated with the development, progression and metastasis of ovarian cancer. In this study, guided by an in-depth analysis of the clinical characteristics of the expression pattern of SIRT2 in ovarian cancer patients, the first SIRT2-targeted hydrophobic tagging (HyT) degraders have been developed. These acyl thiourea degraders exhibited remarkable anti-proliferative activity in several ovarian cancer cells. Among them, the most effective compound Ⅱ-6 exhibited excellent anti-tumor activity both in vitro and in vivo (half maximal inhibitory concentration (IC50) = 0.002 ± 0.001 µmol/L). In addition, Ⅱ-6 was found to effectively suppress cancer cell proliferation and migration, as well as cell cycle arrest and apoptosis. Moreover, further investigation revealed that compound Ⅱ-6 indirectly induced DNA damage through the H4K20me2/53BP1 pathway by degradation of SIRT2. The study not only exemplifies the advantage of the novel HyT degradation strategy but also prove the great potential of SIRT2 as a promising target for drug development of ovarian cancer.
Sirtuin 2 (SIRT2) is one of the key members of sirtuins family that plays important role in regulating many physiological processes. Recent evidences have revealed that SIRT2 is associated with the development, progression and metastasis of ovarian cancer. In this study, guided by an in-depth analysis of the clinical characteristics of the expression pattern of SIRT2 in ovarian cancer patients, the first SIRT2-targeted hydrophobic tagging (HyT) degraders have been developed. These acyl thiourea degraders exhibited remarkable anti-proliferative activity in several ovarian cancer cells. Among them, the most effective compound Ⅱ-6 exhibited excellent anti-tumor activity both in vitro and in vivo (half maximal inhibitory concentration (IC50) = 0.002 ± 0.001 µmol/L). In addition, Ⅱ-6 was found to effectively suppress cancer cell proliferation and migration, as well as cell cycle arrest and apoptosis. Moreover, further investigation revealed that compound Ⅱ-6 indirectly induced DNA damage through the H4K20me2/53BP1 pathway by degradation of SIRT2. The study not only exemplifies the advantage of the novel HyT degradation strategy but also prove the great potential of SIRT2 as a promising target for drug development of ovarian cancer.
2026, 37(4): 111144
doi: 10.1016/j.cclet.2025.111144
Abstract:
The vast majority of lanthanide-doped nanoparticles (LnNPs) exhibit a single mode of upconversion luminescence (UCL) or downshifting luminescence (DSL) for photodynamic therapy (PDT) or diagnostic imaging of tumors, respectively. In order to achieve both UCL and DSL, it is often necessary to dope the luminescent ions in different shell layers to prevent their luminescence quenching, resulting in tedious synthesis steps. Herein, upconversion-downshifting nanoparticles (UDNPs) co-doped with Er3+ and Ho3+ enable the simultaneous dual-wavelength DSL for in vivo near-infrared (NIR)-Ⅱ fluorescence imaging of tumors. On the other hand, the UCL of UDNPs could activate merocyanine photosensitizers (MC 540), resulting in the generation of reactive oxygen species (ROS) and the achievement of PDT. Importantly, Au NPs with glucose oxidase-like properties could consume glucose and promote H2O2 accumulation in tumor cells. Au-catalyzed UDNPs modified with Fe-tannic acid (FeTA) (UDNP-MC/Au-FeTA) could not only enhance the effect of PDT but also realize chemodynamic therapy (CDT) by reacting with Fe2+ generated from slightly acidic decomposition of FeTA to accelerate hydroxyl radical (•OH) generation. The combination of long- and short-acting dual-dynamic therapy could mutually reinforce and compensate for the lack of therapeutic efficacy resulting from luminescence quenching caused by co-doping luminescent ions. Therefore, UDNP-MC/Au-FeTA guided by NIR-Ⅱ fluorescence imaging could achieve efficient synergistic dual-dynamic therapy of tumors through differentially expressed genes associated with apoptosis and oxidative stress-related pathways. NIR-Ⅱ fluorescence imaging diagnostic and dual-dynamic therapeutic strategy, which employs Au-catalyzed lanthanide co-doped UDNPs represents a dexterous design concept for promising anti-tumor applications.
The vast majority of lanthanide-doped nanoparticles (LnNPs) exhibit a single mode of upconversion luminescence (UCL) or downshifting luminescence (DSL) for photodynamic therapy (PDT) or diagnostic imaging of tumors, respectively. In order to achieve both UCL and DSL, it is often necessary to dope the luminescent ions in different shell layers to prevent their luminescence quenching, resulting in tedious synthesis steps. Herein, upconversion-downshifting nanoparticles (UDNPs) co-doped with Er3+ and Ho3+ enable the simultaneous dual-wavelength DSL for in vivo near-infrared (NIR)-Ⅱ fluorescence imaging of tumors. On the other hand, the UCL of UDNPs could activate merocyanine photosensitizers (MC 540), resulting in the generation of reactive oxygen species (ROS) and the achievement of PDT. Importantly, Au NPs with glucose oxidase-like properties could consume glucose and promote H2O2 accumulation in tumor cells. Au-catalyzed UDNPs modified with Fe-tannic acid (FeTA) (UDNP-MC/Au-FeTA) could not only enhance the effect of PDT but also realize chemodynamic therapy (CDT) by reacting with Fe2+ generated from slightly acidic decomposition of FeTA to accelerate hydroxyl radical (•OH) generation. The combination of long- and short-acting dual-dynamic therapy could mutually reinforce and compensate for the lack of therapeutic efficacy resulting from luminescence quenching caused by co-doping luminescent ions. Therefore, UDNP-MC/Au-FeTA guided by NIR-Ⅱ fluorescence imaging could achieve efficient synergistic dual-dynamic therapy of tumors through differentially expressed genes associated with apoptosis and oxidative stress-related pathways. NIR-Ⅱ fluorescence imaging diagnostic and dual-dynamic therapeutic strategy, which employs Au-catalyzed lanthanide co-doped UDNPs represents a dexterous design concept for promising anti-tumor applications.
2026, 37(4): 111145
doi: 10.1016/j.cclet.2025.111145
Abstract:
Accurate cancer diagnosis is essential for fluorescence surgical navigation to eliminate tumors. Second near-infrared (NIR-Ⅱ, 1000–1700 nm) probes with aggregation-induced emission (AIE) nature possess bright fluorescence in a biological environment. However, due to the large particle sizes, NIR-Ⅱ AIE probes usually lead to high liver retention, which is not conducive to tumor enrichment. Therefore, this work constructs a novel amphiphilic NIR-Ⅱ AIE molecule, TTB-PEG1000, which can self-assemble into ultra-small fluorescent dots (7 nm) in the aqueous environment with a maximum emission at 1080 nm. Based on its excellent photostability, morphological stability, and biocompatibility, TTB-PEG1000 shows a desirable definition of angiography capability with high signal-to-background (SBR) in the NIR-Ⅱ AIE window over 1300 nm. Notably, treatment with TTB-PEG1000 in the glioma-tumor mice results in a significant enhancement of the accumulation in the tumor and reduction of the retention in the liver, in which the fluorescent ratio between tumor and liver (T/L) is 32-fold higher than that of their contrast (TTB-COOH NPs) prepared by the nanoprecipitation method. This work is the first report of an amphiphilic AIE molecule with NIR-Ⅱ maximum emission and sub-10 nm size, which will promise for preclinical applications and inspire further exploration of NIR-Ⅱ fluorophores for advanced biomedical imaging.
Accurate cancer diagnosis is essential for fluorescence surgical navigation to eliminate tumors. Second near-infrared (NIR-Ⅱ, 1000–1700 nm) probes with aggregation-induced emission (AIE) nature possess bright fluorescence in a biological environment. However, due to the large particle sizes, NIR-Ⅱ AIE probes usually lead to high liver retention, which is not conducive to tumor enrichment. Therefore, this work constructs a novel amphiphilic NIR-Ⅱ AIE molecule, TTB-PEG1000, which can self-assemble into ultra-small fluorescent dots (7 nm) in the aqueous environment with a maximum emission at 1080 nm. Based on its excellent photostability, morphological stability, and biocompatibility, TTB-PEG1000 shows a desirable definition of angiography capability with high signal-to-background (SBR) in the NIR-Ⅱ AIE window over 1300 nm. Notably, treatment with TTB-PEG1000 in the glioma-tumor mice results in a significant enhancement of the accumulation in the tumor and reduction of the retention in the liver, in which the fluorescent ratio between tumor and liver (T/L) is 32-fold higher than that of their contrast (TTB-COOH NPs) prepared by the nanoprecipitation method. This work is the first report of an amphiphilic AIE molecule with NIR-Ⅱ maximum emission and sub-10 nm size, which will promise for preclinical applications and inspire further exploration of NIR-Ⅱ fluorophores for advanced biomedical imaging.
2026, 37(4): 111161
doi: 10.1016/j.cclet.2025.111161
Abstract:
Penispirolactam (1) and penipyrroloindole (2), two highly modified paspaline-type indole diterpenoids (IDTs), along with three new (3–5) and two known (6 and 7) paspaline-type IDTs were obtained from the endophytic fungus Penicillium janthinellum H-6 guided by liquid chromatography-mass spectrometry (LC-MS)-based molecular network. Architecturally, penispirolactam (1) possesses a unique octacyclic skeleton (6/5/6/6/5/6/6/6) with a spiro core formed by the integration of a C6–C2 unit with the indole moiety, and penipyrroloindole (2) represents a rearranged octacyclic skeleton (6/5/6/5/5/6/6/6) with a pyrrolo[1,2-a]indole core fragment. Their structures, including absolute configurations, were established by detailed spectroscopic analysis, gauge-independent atomic orbital (GIAO) 1D nuclear magnetic resonance (NMR) (DP4+) calculation protocol, and electronic circular dichroism (ECD) calculation method. The plausible biosynthetic pathway of compounds 1 and 2 was also speculated. Additionally, the anti-hepatic fibrosis activity of all compounds was explored, and it was found that 1 could exert its effects by inhibiting the transforming growth factor-β (TGF-β)/Smad signaling pathway without cytotoxicity.
Penispirolactam (1) and penipyrroloindole (2), two highly modified paspaline-type indole diterpenoids (IDTs), along with three new (3–5) and two known (6 and 7) paspaline-type IDTs were obtained from the endophytic fungus Penicillium janthinellum H-6 guided by liquid chromatography-mass spectrometry (LC-MS)-based molecular network. Architecturally, penispirolactam (1) possesses a unique octacyclic skeleton (6/5/6/6/5/6/6/6) with a spiro core formed by the integration of a C6–C2 unit with the indole moiety, and penipyrroloindole (2) represents a rearranged octacyclic skeleton (6/5/6/5/5/6/6/6) with a pyrrolo[1,2-a]indole core fragment. Their structures, including absolute configurations, were established by detailed spectroscopic analysis, gauge-independent atomic orbital (GIAO) 1D nuclear magnetic resonance (NMR) (DP4+) calculation protocol, and electronic circular dichroism (ECD) calculation method. The plausible biosynthetic pathway of compounds 1 and 2 was also speculated. Additionally, the anti-hepatic fibrosis activity of all compounds was explored, and it was found that 1 could exert its effects by inhibiting the transforming growth factor-β (TGF-β)/Smad signaling pathway without cytotoxicity.
2026, 37(4): 111163
doi: 10.1016/j.cclet.2025.111163
Abstract:
Up to now, aggregation-induced emission (AIE) and aggregation-caused quenching (ACQ) have been widely used for fluorescence sensing, respectively. In our study, we covalently linked cyanine dye and 2-cyanobenzothiazole (CBT) to construct fluorescent probe NPCS. Through spectroscopic testing, it was found that the probe itself has both AIE and ACQ behavior. And these acts are borne by CBT and cyanine (CY) respectively. In this study, it was found that glutathione (GSH) showed aggregation and disaggregation effects on two parts of the probe, namely: low concentration of GSH mainly aggravated AIE, and high concentration of GSH disaggregated ACQ of the probe, both of which led to fluorescence enhancement effect and achieved turn-on fluorescence detection of high and low concentrations of GSH. Cysteine (Cys), on the other hand, can undergo a click reaction with the cyano group to generate a stable fluorescent signal. Since Cys does not have the ability to disaggregate, the probe can achieve non-competitive discrimination detection of Cys and GSH. Real-time discriminatory detection of changes in Cys and GSH levels was demonstrated in living cells. The results of this study provide a new perspective for the development of emerging recognition mechanisms and multi-functionality of probes.
Up to now, aggregation-induced emission (AIE) and aggregation-caused quenching (ACQ) have been widely used for fluorescence sensing, respectively. In our study, we covalently linked cyanine dye and 2-cyanobenzothiazole (CBT) to construct fluorescent probe NPCS. Through spectroscopic testing, it was found that the probe itself has both AIE and ACQ behavior. And these acts are borne by CBT and cyanine (CY) respectively. In this study, it was found that glutathione (GSH) showed aggregation and disaggregation effects on two parts of the probe, namely: low concentration of GSH mainly aggravated AIE, and high concentration of GSH disaggregated ACQ of the probe, both of which led to fluorescence enhancement effect and achieved turn-on fluorescence detection of high and low concentrations of GSH. Cysteine (Cys), on the other hand, can undergo a click reaction with the cyano group to generate a stable fluorescent signal. Since Cys does not have the ability to disaggregate, the probe can achieve non-competitive discrimination detection of Cys and GSH. Real-time discriminatory detection of changes in Cys and GSH levels was demonstrated in living cells. The results of this study provide a new perspective for the development of emerging recognition mechanisms and multi-functionality of probes.
2026, 37(4): 111166
doi: 10.1016/j.cclet.2025.111166
Abstract:
As fundamental chemicals, alkynes have been pivotal in synthesizing numerous value-added compounds. Direct manipulation of alkynes offers rapid access to diverse chemical spaces. Cleaving the alkyne triple bond has traditionally required harsh conditions due to its high bond dissociation energy. Here, we present a manganese-catalyzed electrochemical nitrogenation method for the direct cleavage of C≡C bonds, efficiently generating various nitriles under mild conditions. This reaction demonstrates extensive functional group tolerance and eliminates the need for stoichiometric chemical oxidants. CV experiments verified the role of Mn catalysis, and the N3 radical intermediate was confirmed by EPR spectroscopy. Our synthetic protocol provides a promising and versatile alternative for constructing nitrogen-containing compounds, potentially transforming approaches in chemical synthesis
As fundamental chemicals, alkynes have been pivotal in synthesizing numerous value-added compounds. Direct manipulation of alkynes offers rapid access to diverse chemical spaces. Cleaving the alkyne triple bond has traditionally required harsh conditions due to its high bond dissociation energy. Here, we present a manganese-catalyzed electrochemical nitrogenation method for the direct cleavage of C≡C bonds, efficiently generating various nitriles under mild conditions. This reaction demonstrates extensive functional group tolerance and eliminates the need for stoichiometric chemical oxidants. CV experiments verified the role of Mn catalysis, and the N3 radical intermediate was confirmed by EPR spectroscopy. Our synthetic protocol provides a promising and versatile alternative for constructing nitrogen-containing compounds, potentially transforming approaches in chemical synthesis
2026, 37(4): 111167
doi: 10.1016/j.cclet.2025.111167
Abstract:
Amino acids are the building blocks of proteins and various bioactive molecules. Fluorination is a key strategy in medicinal chemistry, making the development of new and efficient methods for fluorinating amino acids highly desirable. While many fluorination reagents have been developed, their application on amino acid frameworks remains limited. In this study, we demonstrate that ethyl 3-bromo-2-((diphenylmethylene)amino)-3,3-difluoropropanoate is an effective gem-difluoroalkenes precursor for constructing a library of monofluoroolefin amino acids via a Pd-catalyzed cross-coupling reaction.
Amino acids are the building blocks of proteins and various bioactive molecules. Fluorination is a key strategy in medicinal chemistry, making the development of new and efficient methods for fluorinating amino acids highly desirable. While many fluorination reagents have been developed, their application on amino acid frameworks remains limited. In this study, we demonstrate that ethyl 3-bromo-2-((diphenylmethylene)amino)-3,3-difluoropropanoate is an effective gem-difluoroalkenes precursor for constructing a library of monofluoroolefin amino acids via a Pd-catalyzed cross-coupling reaction.
2026, 37(4): 111171
doi: 10.1016/j.cclet.2025.111171
Abstract:
Orthogonal molecular orbitals (MOs) of donor-acceptor (D-A) pairs favor the spin-orbit charge transfer intersystem crossing (SOCT-ISC) transition, and herein 2-anthryl asymmetric aza-boradiazaindacene (aza-BODIPY) (AH-BDP) was designed and prepared. According to the X-ray crystallography, the steric hindrance in orthogonal molecule AH-BDP results in a large dihedral angle between the two MO planes. Since low ΔEst prefers to undertake ISC and efficiently produce reactive oxygen species (ROS), the calculated ΔEst for AH-BDP is 0.757 eV, significantly smaller than that of the aza-BDOPY without anthryl group DH-BDP (1.052 eV). AH-BDP as a heavy-atom-free photosensitizer not only produced the singlet oxygen, but also possessed photothermal conversion efficiency. Self-assembly AH-BDP nanoparticles (NPs) could efficiently induce HCT116 cells elimination in nude mice through ROS/heat-mediated pathways.
Orthogonal molecular orbitals (MOs) of donor-acceptor (D-A) pairs favor the spin-orbit charge transfer intersystem crossing (SOCT-ISC) transition, and herein 2-anthryl asymmetric aza-boradiazaindacene (aza-BODIPY) (AH-BDP) was designed and prepared. According to the X-ray crystallography, the steric hindrance in orthogonal molecule AH-BDP results in a large dihedral angle between the two MO planes. Since low ΔEst prefers to undertake ISC and efficiently produce reactive oxygen species (ROS), the calculated ΔEst for AH-BDP is 0.757 eV, significantly smaller than that of the aza-BDOPY without anthryl group DH-BDP (1.052 eV). AH-BDP as a heavy-atom-free photosensitizer not only produced the singlet oxygen, but also possessed photothermal conversion efficiency. Self-assembly AH-BDP nanoparticles (NPs) could efficiently induce HCT116 cells elimination in nude mice through ROS/heat-mediated pathways.
2026, 37(4): 111172
doi: 10.1016/j.cclet.2025.111172
Abstract:
Alzheimer's disease (AD) is a complex and multifactorial neurodegenerative disorder, marked by a variety of pathological hallmarks such as oxidative stress (OS), metal accumulation, and the aggregation of amyloid-beta (Aβ) proteins. Erucin, a natural compound present in cruciferous plants, has demonstrated promising therapeutic potential in modulating neurodegenerative diseases, hinting at its neuroprotective capabilities. In this study, we engineered an innovative intracellular protein delivery system centered around erucin. This delivery platform operates through a cell membrane perforation mechanism, enabling the swift translocation of target proteins into the cytoplasm. As a result, it substantially shortens the time required for the proteins to exert their functions. Significantly, this delivery system inherently possesses the capacity to inhibit Aβ aggregation. In PC12 cell models, the delivery of the antioxidant enzyme superoxide dismutase (SOD) successfully mitigated the OS triggered by Aβ aggregation and decreased cytotoxicity. This multifaceted therapeutic strategy holds great promise as an effective approach for the treatment of AD.
Alzheimer's disease (AD) is a complex and multifactorial neurodegenerative disorder, marked by a variety of pathological hallmarks such as oxidative stress (OS), metal accumulation, and the aggregation of amyloid-beta (Aβ) proteins. Erucin, a natural compound present in cruciferous plants, has demonstrated promising therapeutic potential in modulating neurodegenerative diseases, hinting at its neuroprotective capabilities. In this study, we engineered an innovative intracellular protein delivery system centered around erucin. This delivery platform operates through a cell membrane perforation mechanism, enabling the swift translocation of target proteins into the cytoplasm. As a result, it substantially shortens the time required for the proteins to exert their functions. Significantly, this delivery system inherently possesses the capacity to inhibit Aβ aggregation. In PC12 cell models, the delivery of the antioxidant enzyme superoxide dismutase (SOD) successfully mitigated the OS triggered by Aβ aggregation and decreased cytotoxicity. This multifaceted therapeutic strategy holds great promise as an effective approach for the treatment of AD.
2026, 37(4): 111174
doi: 10.1016/j.cclet.2025.111174
Abstract:
Aqueous zinc-ion batteries (AZIBs) have drawn numerous attention due to their low cost and environmental benefits. However, its commercialization process was hindered by issues, such as uncontrolled dendrite growth and parasitic side reactions. Inspired by the natural interaction between Zn2+ and amino acid chains in zinc finger proteins, we introduced L-proline (LP), a cost-effective additive, into the aqueous electrolyte to stabilize the Zn anode. In combination with experiments and theoretical calculation results, it is demonstrated that the LP additive tends to reshape the hydrated Zn2+ solvation sheath and weaken the free H2O activity, thereby restricting the water-induced parasitic reactions and drastic dendrite growth. Therefore, the Zn symmetrical cells with LP-containing electrolytes delivered an excellent superior electrochemical performance, including a long-term calendar lifespan of 3400 h at 2 mA/cm2 and nearly 450 h at 5 mA/cm2. Meanwhile, the as-assembled Zn||MnO2 full cells also showed desired cycling stability and rate performance with the assistance of LP additive, outperforming the ZnSO4 system. This intriguing bio-inspired strategy provides a valuable insight for improving the longevity of AZIBs and advancing their development in energy storage.
Aqueous zinc-ion batteries (AZIBs) have drawn numerous attention due to their low cost and environmental benefits. However, its commercialization process was hindered by issues, such as uncontrolled dendrite growth and parasitic side reactions. Inspired by the natural interaction between Zn2+ and amino acid chains in zinc finger proteins, we introduced L-proline (LP), a cost-effective additive, into the aqueous electrolyte to stabilize the Zn anode. In combination with experiments and theoretical calculation results, it is demonstrated that the LP additive tends to reshape the hydrated Zn2+ solvation sheath and weaken the free H2O activity, thereby restricting the water-induced parasitic reactions and drastic dendrite growth. Therefore, the Zn symmetrical cells with LP-containing electrolytes delivered an excellent superior electrochemical performance, including a long-term calendar lifespan of 3400 h at 2 mA/cm2 and nearly 450 h at 5 mA/cm2. Meanwhile, the as-assembled Zn||MnO2 full cells also showed desired cycling stability and rate performance with the assistance of LP additive, outperforming the ZnSO4 system. This intriguing bio-inspired strategy provides a valuable insight for improving the longevity of AZIBs and advancing their development in energy storage.
2026, 37(4): 111175
doi: 10.1016/j.cclet.2025.111175
Abstract:
Aqueous zinc-ion hybrid capacitors (AZICs) combine the advantageous characteristics of the high energy density of aqueous zinc-ion batteries with the high power density of supercapacitors. However, their practical application is limited by the instability of the zinc anode and the relatively low capacity of the carbon cathode. To address these challenges, we propose the utilization of p-benzoquinone (BQ) as a bifunctional electrolyte additive. This additive adsorbs onto the zinc surface and modifies the Zn2+ solvation structure, effectively suppressing the growth of zinc dendrites and mitigating water-related side reactions. As a result, the lifespan of the zinc anode is significantly extended from 35 h to 1188 h at 0.5 mA/cm2 and 0.5 mAh/cm2, with a high average Coulombic efficiency of 99.30%. Additionally, the BQ additive enhances the specific capacity of the cathode through its rapid redox reactions on the cathode surface. The AZIC also demonstrates a notable increase in capacity, rising from 40 mAh/g to 140 mAh/g at 0.5 A/g, alongside improved rate performance and cycling stability. This study offers an efficient strategy to simultaneously address the stability and energy density limitations of AZICs.
Aqueous zinc-ion hybrid capacitors (AZICs) combine the advantageous characteristics of the high energy density of aqueous zinc-ion batteries with the high power density of supercapacitors. However, their practical application is limited by the instability of the zinc anode and the relatively low capacity of the carbon cathode. To address these challenges, we propose the utilization of p-benzoquinone (BQ) as a bifunctional electrolyte additive. This additive adsorbs onto the zinc surface and modifies the Zn2+ solvation structure, effectively suppressing the growth of zinc dendrites and mitigating water-related side reactions. As a result, the lifespan of the zinc anode is significantly extended from 35 h to 1188 h at 0.5 mA/cm2 and 0.5 mAh/cm2, with a high average Coulombic efficiency of 99.30%. Additionally, the BQ additive enhances the specific capacity of the cathode through its rapid redox reactions on the cathode surface. The AZIC also demonstrates a notable increase in capacity, rising from 40 mAh/g to 140 mAh/g at 0.5 A/g, alongside improved rate performance and cycling stability. This study offers an efficient strategy to simultaneously address the stability and energy density limitations of AZICs.
2026, 37(4): 111199
doi: 10.1016/j.cclet.2025.111199
Abstract:
The inappropriate use of antibiotics has led to the emergence of drug-resistant bacteria and the formation of persistent biofilms, rendering conventional antibiotics ineffective against these infections. To address this challenge, the enzyme-like activity of nanozymes, particularly those with photothermal effects, is being explored. However, the development of nanozymes is hindered by the complex synthesis processes involved and the consumption of reactive oxygen species (ROS) by reducing products in bacteria. This article presents an interesting strategy utilizing near-infrared laser-enhanced oxidase-like (OXD-like) activity of manganese dioxide nanoparticles (MnO2 NPs) to combat subcutaneous infections caused by methicillin-resistant Staphylococcus aureus (MRSA). MnO2 NPs, characterized by flower-like morphology and broad near-infrared absorption, exhibited favorable OXD-like activity and a stable photothermal effect. Experiments in vitro revealed that the combined high thermal effect and the substantial production of ROS effectively targeted MRSA and disrupted biofilm. The efficacy of MnO2 in vivo was validated through the establishment of a subcutaneous abscess model. Additionally, a series of biosafety tests, including routine blood tests and blood biochemistry analyses, confirmed the safety of MnO2 in vivo. Collectively, these findings suggest that combination therapy involving MnO2 presents a promising therapeutic approach for addressing infections associated with biofilms and drug-resistant bacteria.
The inappropriate use of antibiotics has led to the emergence of drug-resistant bacteria and the formation of persistent biofilms, rendering conventional antibiotics ineffective against these infections. To address this challenge, the enzyme-like activity of nanozymes, particularly those with photothermal effects, is being explored. However, the development of nanozymes is hindered by the complex synthesis processes involved and the consumption of reactive oxygen species (ROS) by reducing products in bacteria. This article presents an interesting strategy utilizing near-infrared laser-enhanced oxidase-like (OXD-like) activity of manganese dioxide nanoparticles (MnO2 NPs) to combat subcutaneous infections caused by methicillin-resistant Staphylococcus aureus (MRSA). MnO2 NPs, characterized by flower-like morphology and broad near-infrared absorption, exhibited favorable OXD-like activity and a stable photothermal effect. Experiments in vitro revealed that the combined high thermal effect and the substantial production of ROS effectively targeted MRSA and disrupted biofilm. The efficacy of MnO2 in vivo was validated through the establishment of a subcutaneous abscess model. Additionally, a series of biosafety tests, including routine blood tests and blood biochemistry analyses, confirmed the safety of MnO2 in vivo. Collectively, these findings suggest that combination therapy involving MnO2 presents a promising therapeutic approach for addressing infections associated with biofilms and drug-resistant bacteria.
2026, 37(4): 111200
doi: 10.1016/j.cclet.2025.111200
Abstract:
An efficient skeletal editing for the construction of 2-benzodiazepines from benzo[c]oxepines was developed through atom-swapping of oxygen atom to the nitrogen atom. This reaction integrated the sequential ring-opening/substitution/ring-closing in the continuous manufacturing one-pot synthesis. The reaction conditions are mild, transition metal-free, simple-operated and the substrates are widely applicable. The anti-tumor activity of some synthesized 2-benzodiazepine compounds shows this atom-swapping skeletal editing through the deconstruction-reconstruction of heterocycles is attractive and effective in the discovery of new drug skeletons.
An efficient skeletal editing for the construction of 2-benzodiazepines from benzo[c]oxepines was developed through atom-swapping of oxygen atom to the nitrogen atom. This reaction integrated the sequential ring-opening/substitution/ring-closing in the continuous manufacturing one-pot synthesis. The reaction conditions are mild, transition metal-free, simple-operated and the substrates are widely applicable. The anti-tumor activity of some synthesized 2-benzodiazepine compounds shows this atom-swapping skeletal editing through the deconstruction-reconstruction of heterocycles is attractive and effective in the discovery of new drug skeletons.
2026, 37(4): 111215
doi: 10.1016/j.cclet.2025.111215
Abstract:
Zinc ions (Zn2+) play a crucial role in maintaining human health, and their imbalance has been associated with various diseases and environmental contamination. Although many fluorescent probes have been developed for Zn2+ detection, they often face challenges, including short emission wavelengths, narrow Stokes shifts, and particularly the poor selectivity. Here, aromatic rings with different electron densities including benzene, thiophene and furan rings, were introduced as aromatic π-conjugated bridges to connect dicyanoisophorone (DCI) and amide-di-2-picolylamine (DPA) based structures, and three probes L1, L2 and L3 for Zn2+ detection were developed. Our results demonstrated that compared with L1, L2 and L3, which inserting thiophene and furan rings, revealed near-infrared (NIR) emission at 651 nm, and a larger Stokes shift of 187 nm. Notably, different from L2, L3, which incorporated a furan ring with the highest electron density, exhibited the highest selectivity for Zn2+ with a low detection limit of 31 nmol/L. In addition, the binding mode of L3 with Zn2+ was confirmed in the form of an imidic acid tautomer. Furthermore, L3 was successfully applied in cellular imaging, validating its potential for in vivo bioimaging. This study presents a promising strategy for developing high-performance Zn2+ probes by simply modifying the aromatic π-conjugated bridges.
Zinc ions (Zn2+) play a crucial role in maintaining human health, and their imbalance has been associated with various diseases and environmental contamination. Although many fluorescent probes have been developed for Zn2+ detection, they often face challenges, including short emission wavelengths, narrow Stokes shifts, and particularly the poor selectivity. Here, aromatic rings with different electron densities including benzene, thiophene and furan rings, were introduced as aromatic π-conjugated bridges to connect dicyanoisophorone (DCI) and amide-di-2-picolylamine (DPA) based structures, and three probes L1, L2 and L3 for Zn2+ detection were developed. Our results demonstrated that compared with L1, L2 and L3, which inserting thiophene and furan rings, revealed near-infrared (NIR) emission at 651 nm, and a larger Stokes shift of 187 nm. Notably, different from L2, L3, which incorporated a furan ring with the highest electron density, exhibited the highest selectivity for Zn2+ with a low detection limit of 31 nmol/L. In addition, the binding mode of L3 with Zn2+ was confirmed in the form of an imidic acid tautomer. Furthermore, L3 was successfully applied in cellular imaging, validating its potential for in vivo bioimaging. This study presents a promising strategy for developing high-performance Zn2+ probes by simply modifying the aromatic π-conjugated bridges.
2026, 37(4): 111217
doi: 10.1016/j.cclet.2025.111217
Abstract:
Density functional theory calculations were performed to investigate the iridium-catalyzed atroposelective intermolecular C-H silylation of 2-arylisoquinolines. The Ir(Ⅲ) hydride species was identified as the active catalyst species of the reaction. The computations show that the reaction occurs through the Ir(Ⅲ)/Ir(V) catalytic cycle. The C(sp2)-H oxidative addition represents the rate- and enantioselectivity-determining step. The distortion/interaction and structural analyses reveal that the BINEPINE skeleton of the PSiSi ligand creates an axially chiral pocket for the C-H oxidative addition, providing a ligand-enabled axial chirality transfer strategy responsible for the observed enantioselectivity. The match/mismatch in axial chirality between reacting 2-arylisoquinolines and the BINEPINE skeleton of the PSiSi ligand plays a key role in governing enantioselectivity.
Density functional theory calculations were performed to investigate the iridium-catalyzed atroposelective intermolecular C-H silylation of 2-arylisoquinolines. The Ir(Ⅲ) hydride species was identified as the active catalyst species of the reaction. The computations show that the reaction occurs through the Ir(Ⅲ)/Ir(V) catalytic cycle. The C(sp2)-H oxidative addition represents the rate- and enantioselectivity-determining step. The distortion/interaction and structural analyses reveal that the BINEPINE skeleton of the PSiSi ligand creates an axially chiral pocket for the C-H oxidative addition, providing a ligand-enabled axial chirality transfer strategy responsible for the observed enantioselectivity. The match/mismatch in axial chirality between reacting 2-arylisoquinolines and the BINEPINE skeleton of the PSiSi ligand plays a key role in governing enantioselectivity.
2026, 37(4): 111220
doi: 10.1016/j.cclet.2025.111220
Abstract:
Ferroptosis has emerged as a significant pathway in various pathological conditions. Studying the effects of inhibiting ferroptosis on liver injury is instrumental in gaining a deeper understanding of the mechanisms. This study the design and synthesis of a multi-channel near-infrared emitting fluorescent probe TXVQ. When the probe TXVQ responds to HSO3−, the fluorescence intensity at 500 nm of TXVQ increases with the addition of HSO3−. As the concentration of H2O2 increases, the fluorescence intensity of TXVQ at 600 nm is enhanced. Concurrently, as viscosity rises, the fluorescence intensity of the probe TXVQ at 725 nm will gradually increase. The probe TXVQ, with its ability to monitor HSO3−, H2O2 and viscosity through three distinct fluorescent channels, is advantageous for its application in the biological field. Subsequently, cellular experiments have demonstrated that the probe TXVQ can monitor changes in intracellular HSO3−, H2O2 and viscosity. At the cellular level, it is found that inhibiting ferroptosis had no alleviating effect on drug-induced liver injury (DILI), but it had a certain alleviating effect on acute kidney injury (AKI). In a murine model, the effects of ferroptosis inhibition on DILI and AKI indicate that inhibiting ferroptosis reduced kidney injury but not liver injury, highlighting its potential in kidney therapeutics. TXVQ can detect various levels of HSO3−, H2O2 and viscosity through three different fluorescent channels, making it a powerful tool for diagnosing and treating kidney diseases, as well as deepening the understanding of the role of ferroptosis in liver and kidney pathologies.
Ferroptosis has emerged as a significant pathway in various pathological conditions. Studying the effects of inhibiting ferroptosis on liver injury is instrumental in gaining a deeper understanding of the mechanisms. This study the design and synthesis of a multi-channel near-infrared emitting fluorescent probe TXVQ. When the probe TXVQ responds to HSO3−, the fluorescence intensity at 500 nm of TXVQ increases with the addition of HSO3−. As the concentration of H2O2 increases, the fluorescence intensity of TXVQ at 600 nm is enhanced. Concurrently, as viscosity rises, the fluorescence intensity of the probe TXVQ at 725 nm will gradually increase. The probe TXVQ, with its ability to monitor HSO3−, H2O2 and viscosity through three distinct fluorescent channels, is advantageous for its application in the biological field. Subsequently, cellular experiments have demonstrated that the probe TXVQ can monitor changes in intracellular HSO3−, H2O2 and viscosity. At the cellular level, it is found that inhibiting ferroptosis had no alleviating effect on drug-induced liver injury (DILI), but it had a certain alleviating effect on acute kidney injury (AKI). In a murine model, the effects of ferroptosis inhibition on DILI and AKI indicate that inhibiting ferroptosis reduced kidney injury but not liver injury, highlighting its potential in kidney therapeutics. TXVQ can detect various levels of HSO3−, H2O2 and viscosity through three different fluorescent channels, making it a powerful tool for diagnosing and treating kidney diseases, as well as deepening the understanding of the role of ferroptosis in liver and kidney pathologies.
2026, 37(4): 111225
doi: 10.1016/j.cclet.2025.111225
Abstract:
In this study, we report a palladium-catalyzed carbene C-H insertion reaction of non-activated arenes using N-tosylhydrazones as both carbene and olefin precursors. This method consists of a two-step, one-pot process, where the arenes are first thianthrenated and then undergo migratory insertion/β-H elimination with N-tosylhydrazones to form aryl alkenes. This highly site-selective C-H alkenylation of arenes demonstrates a relatively broad substrate scope and exhibits high tolerance for halogen substituents. Importantly, this transformation allows for the modification of the arene moiety in commercially available bioactive molecules, underscoring its significant potential for late-stage functionalization of arene-containing pharmaceuticals.
In this study, we report a palladium-catalyzed carbene C-H insertion reaction of non-activated arenes using N-tosylhydrazones as both carbene and olefin precursors. This method consists of a two-step, one-pot process, where the arenes are first thianthrenated and then undergo migratory insertion/β-H elimination with N-tosylhydrazones to form aryl alkenes. This highly site-selective C-H alkenylation of arenes demonstrates a relatively broad substrate scope and exhibits high tolerance for halogen substituents. Importantly, this transformation allows for the modification of the arene moiety in commercially available bioactive molecules, underscoring its significant potential for late-stage functionalization of arene-containing pharmaceuticals.
2026, 37(4): 111235
doi: 10.1016/j.cclet.2025.111235
Abstract:
Colon cancer is one of the malignant tumors with high morbidity and mortality worldwide, and its etiology is closely related to high levels of hydrogen sulfide (H2S). To date, H2S-activated near-infrared (NIR) fluorescent (FL) probes with high tumor tropism are still scarce. In this work, we created a new NIR FL probes (Cy-DG) that enables colon cancer targeted imaging and rapid fecal optical analysis by introducing an H2S-recognition moiety and two D-glucosamine fragments on the scaffold of QCy7. Cy-DG exhibits excellent properties, including specific "off-on" response toward H2S, intense NIR emission at 703 nm, large Stokes shift (118 nm), and high sensitivity (limit of detection (LOD), 0.48 µmol/L). Notably, the presence of D-glucosamine allows Cy-DG to be preferentially taken up by cancer cells. After intravenous administration, Cy-DG was able to efficiently accumulate in a MC38 intestinal cancer model and sensitively detect endogenous H2S in vivo, showing 5.94-fold higher fluorescence intensity in small tumors < 5 mm. Furthermore, Cy-DG was successfully used to detect H2S in feces samples from colon cancer-bearing mice. We believe that Cy-DG has great potential as a powerful diagnostic tool for H2S-related disorder and stool examinations in the future.
Colon cancer is one of the malignant tumors with high morbidity and mortality worldwide, and its etiology is closely related to high levels of hydrogen sulfide (H2S). To date, H2S-activated near-infrared (NIR) fluorescent (FL) probes with high tumor tropism are still scarce. In this work, we created a new NIR FL probes (Cy-DG) that enables colon cancer targeted imaging and rapid fecal optical analysis by introducing an H2S-recognition moiety and two D-glucosamine fragments on the scaffold of QCy7. Cy-DG exhibits excellent properties, including specific "off-on" response toward H2S, intense NIR emission at 703 nm, large Stokes shift (118 nm), and high sensitivity (limit of detection (LOD), 0.48 µmol/L). Notably, the presence of D-glucosamine allows Cy-DG to be preferentially taken up by cancer cells. After intravenous administration, Cy-DG was able to efficiently accumulate in a MC38 intestinal cancer model and sensitively detect endogenous H2S in vivo, showing 5.94-fold higher fluorescence intensity in small tumors < 5 mm. Furthermore, Cy-DG was successfully used to detect H2S in feces samples from colon cancer-bearing mice. We believe that Cy-DG has great potential as a powerful diagnostic tool for H2S-related disorder and stool examinations in the future.
2026, 37(4): 111250
doi: 10.1016/j.cclet.2025.111250
Abstract:
The single-electron transfer-induced oxidative transformation of indoles has been extensively explored in recent years. However, research toward high enantioselective control in this reaction is rare. Herein, we report an enantioselective catalytic single-electron transfer-induced oxidative rearrangement of cyclic indoles enabled by dual chiral copper/phosphoric acid catalysis. Using atmospheric oxygen (O2) as the terminal oxidant, the reactions of tetrahydro-β-carbolines, tetrahydropyrano[3,4-b]indoles and the challenging tetrahydrocarbazoles are all realized, providing diverse rearrangement products including pyrrolidinyl-, tetrahydrofuranyl- and cyclopentyl-bearing spiroindolinones in good yields with high enantioselectivities. The synthetic utility of this protocol was demonstrated in a concise synthesis of (+)-coerulescine and (+)-horsfiline. These findings would provide new insights and opportunities for future asymmetric oxidative radical reaction design.
The single-electron transfer-induced oxidative transformation of indoles has been extensively explored in recent years. However, research toward high enantioselective control in this reaction is rare. Herein, we report an enantioselective catalytic single-electron transfer-induced oxidative rearrangement of cyclic indoles enabled by dual chiral copper/phosphoric acid catalysis. Using atmospheric oxygen (O2) as the terminal oxidant, the reactions of tetrahydro-β-carbolines, tetrahydropyrano[3,4-b]indoles and the challenging tetrahydrocarbazoles are all realized, providing diverse rearrangement products including pyrrolidinyl-, tetrahydrofuranyl- and cyclopentyl-bearing spiroindolinones in good yields with high enantioselectivities. The synthetic utility of this protocol was demonstrated in a concise synthesis of (+)-coerulescine and (+)-horsfiline. These findings would provide new insights and opportunities for future asymmetric oxidative radical reaction design.
2026, 37(4): 111259
doi: 10.1016/j.cclet.2025.111259
Abstract:
Available online-The enantioselective chlorination is a continuing challenge owing to the highly reactive nature of chloronium ions. Herein, tertiary ammonium salt catalysis for asymmetric chloro– and selenocyclization of 2-alkenyl anilides with high enantioselectivities were achieved at room temperature. This approach affords the green and atom-economical access to chiral 4H-3,1-benzoxazines with excellent functional-group tolerance. The catalyst could be reused for 3 runs, no obvious loss in catalytic activity and enantioselectivity was observed. This catalytic system can be applied to late-stage modification of pharmaceuticals and natural products. Computational mechanistic studies revealed that the non-classical hydrogen bond (C-H…O) between the phosphate anion and ammonium cation plays crucial role in the stereocontrol of the reaction.
Available online-The enantioselective chlorination is a continuing challenge owing to the highly reactive nature of chloronium ions. Herein, tertiary ammonium salt catalysis for asymmetric chloro– and selenocyclization of 2-alkenyl anilides with high enantioselectivities were achieved at room temperature. This approach affords the green and atom-economical access to chiral 4H-3,1-benzoxazines with excellent functional-group tolerance. The catalyst could be reused for 3 runs, no obvious loss in catalytic activity and enantioselectivity was observed. This catalytic system can be applied to late-stage modification of pharmaceuticals and natural products. Computational mechanistic studies revealed that the non-classical hydrogen bond (C-H…O) between the phosphate anion and ammonium cation plays crucial role in the stereocontrol of the reaction.
2026, 37(4): 111276
doi: 10.1016/j.cclet.2025.111276
Abstract:
An efficient method for the three-component azidopyridylation of unactivated alkenes to access β-pyridyl azides has been developed. The overall process involves a visible light-mediated radical-relay sequence that begins with an in situ generated methoxy radical, which may facilitate Si−N3 bond activation to generate azidyl radical under mild conditions. The ensuing azidyl radical adds to the alkenes to furnish the carbon-centered radicals which themselves add, in an intermolecular sense, to pyridinium salts. This three-component photocatalytic strategy is effective for a broad range of alkenes and N-heterocycles, and readily affords synthetically useful azidyl- and pyridyl-containing building blocks. This method provides new insights into methoxy radical-initiated relay reactions as well as access to a range of new molecular scaffolds.
An efficient method for the three-component azidopyridylation of unactivated alkenes to access β-pyridyl azides has been developed. The overall process involves a visible light-mediated radical-relay sequence that begins with an in situ generated methoxy radical, which may facilitate Si−N3 bond activation to generate azidyl radical under mild conditions. The ensuing azidyl radical adds to the alkenes to furnish the carbon-centered radicals which themselves add, in an intermolecular sense, to pyridinium salts. This three-component photocatalytic strategy is effective for a broad range of alkenes and N-heterocycles, and readily affords synthetically useful azidyl- and pyridyl-containing building blocks. This method provides new insights into methoxy radical-initiated relay reactions as well as access to a range of new molecular scaffolds.
2026, 37(4): 111277
doi: 10.1016/j.cclet.2025.111277
Abstract:
Selective activation of C-C bonds via molecular editing is a fundamental challenge in organic synthesis. Among the various strategies, metathesis reactions have emerged as powerful tools for constructing new molecular architectures due to their well-established mechanisms. However, these reactions have largely been limited to the same types of covalent bonds, such as σ-σ or π-π bonds, leaving σ-π cross-metathesis reactions unexplored. Perhaps the bond redistribution between the σ and π bonds is highly difficult due to the lack of p orbital in σ bonds. Herein, we report the first example of a transition metal-free σ-π cross-metathesis reaction that converts methyl ketones into the corresponding carboxylic acids along with the formation of 11H-benzo[b]fluoren-11-one. A comprehensive mechanistic investigation, supported by DFT calculations, was conducted to elucidate the unique reaction pathway. This study not only provides compelling evidence for the first σ-π cross-metathesis reaction but also demonstrates the formation of a key oxetan-2-olate intermediate and its utility in organic transformations. This novel concept and strategy expand the scope of traditional metathesis reactions, offering new possibilities for selective C-C bond activation in a redox-neutral manner.
Selective activation of C-C bonds via molecular editing is a fundamental challenge in organic synthesis. Among the various strategies, metathesis reactions have emerged as powerful tools for constructing new molecular architectures due to their well-established mechanisms. However, these reactions have largely been limited to the same types of covalent bonds, such as σ-σ or π-π bonds, leaving σ-π cross-metathesis reactions unexplored. Perhaps the bond redistribution between the σ and π bonds is highly difficult due to the lack of p orbital in σ bonds. Herein, we report the first example of a transition metal-free σ-π cross-metathesis reaction that converts methyl ketones into the corresponding carboxylic acids along with the formation of 11H-benzo[b]fluoren-11-one. A comprehensive mechanistic investigation, supported by DFT calculations, was conducted to elucidate the unique reaction pathway. This study not only provides compelling evidence for the first σ-π cross-metathesis reaction but also demonstrates the formation of a key oxetan-2-olate intermediate and its utility in organic transformations. This novel concept and strategy expand the scope of traditional metathesis reactions, offering new possibilities for selective C-C bond activation in a redox-neutral manner.
2026, 37(4): 111278
doi: 10.1016/j.cclet.2025.111278
Abstract:
Cell-penetrating peptides (CPPs) hold great potential as a tool using non-invasive delivery of therapeutic or diagnostic molecules into mammalian cells, but their broad application has been limited by poor endosomal escape. Thus, the rational design and selection of CPPs remains a challenge and calls for deeper mechanistic understandings. Here, we developed novel stapled cell-penetrating peptides based on the highly positively charged HIV Tat47-57 peptide using decafluorobiphenyl-cysteine SNAr chemistry which selectively disrupt endosomal membranes. A series of stapled peptides with a cross-linked structure were synthesized and investigated their cellular uptake, endosomal escape and intracellular delivery of cargoes. Among these peptides, analogues P3 and P6 demonstrated the highest cellular uptake and endosomal escape activities with efficiencies 3.5−9-fold higher than that of Tat47-57. Notably, the results demonstrated that the decafluorobiphenyl bridge of stapled peptides exhibited significant ability for cellular uptake and endosomal escape. Moreover, we found that fluorine atoms of decafluorobiphenyl bridge played a key role for disrupting endosomal membranes. Finally, the utility of this strategy has been demonstrated by the intracellular delivery of biomacromolecules (avidin and negatively charged phosphopeptides). Together, these results suggest that the decafluorobiphenyl-cysteine SNAr chemistry may be an efficient strategy for the development of novel stapled CPPs.
Cell-penetrating peptides (CPPs) hold great potential as a tool using non-invasive delivery of therapeutic or diagnostic molecules into mammalian cells, but their broad application has been limited by poor endosomal escape. Thus, the rational design and selection of CPPs remains a challenge and calls for deeper mechanistic understandings. Here, we developed novel stapled cell-penetrating peptides based on the highly positively charged HIV Tat47-57 peptide using decafluorobiphenyl-cysteine SNAr chemistry which selectively disrupt endosomal membranes. A series of stapled peptides with a cross-linked structure were synthesized and investigated their cellular uptake, endosomal escape and intracellular delivery of cargoes. Among these peptides, analogues P3 and P6 demonstrated the highest cellular uptake and endosomal escape activities with efficiencies 3.5−9-fold higher than that of Tat47-57. Notably, the results demonstrated that the decafluorobiphenyl bridge of stapled peptides exhibited significant ability for cellular uptake and endosomal escape. Moreover, we found that fluorine atoms of decafluorobiphenyl bridge played a key role for disrupting endosomal membranes. Finally, the utility of this strategy has been demonstrated by the intracellular delivery of biomacromolecules (avidin and negatively charged phosphopeptides). Together, these results suggest that the decafluorobiphenyl-cysteine SNAr chemistry may be an efficient strategy for the development of novel stapled CPPs.
2026, 37(4): 111279
doi: 10.1016/j.cclet.2025.111279
Abstract:
Hierarchical assembly provides a rational procedure to acquire complex supramolecular architectures from basic building blocks. In this work, a novel kind of double-stranded polyrotaxane motif was reported by Ag+-directed coordination-driven assembly following the preassembly of a four-connected pseudorotaxane (cpb)2CB8 linker. Moreover, supramolecular isomerism is observed in crystalline compounds based on double-stranded polyrotaxane motifs due to differences in lattice stacking mode. Interestingly, the resultant supramolecular isomers, cross-Ag-DSP-1 and para-Ag-DSP-1, show dual thermo- and anion-responsiveness. Benefiting from high crystallinity of these coordination assemblies, a combination of characterization techniques, especially X-ray diffraction, was used to unveil precise molecular mechanisms related to the inherent dynamic behavior of these assemblies, which can be attributed to remarkable lattice rearrangement and crystal transformations as temperature increases or after anion exchange, reflecting the adaptive adjustment ability of these supramolecular architectures in response to external stimuli. Based on the anion exchange capability, these two supramolecular materials show fast removal kinetics and high sorption capacity for perrhenate (ReO4-) anion, a surrogate of radioactive pertechnetate (TcO4-) in nuclear waste eluents. This work provides a feasible way to supramolecular assemblies with customized structures and stimuli-responsiveness, and is helpful to design and synthesize more functional supramolecular systems with complex structures and tailored functions.
Hierarchical assembly provides a rational procedure to acquire complex supramolecular architectures from basic building blocks. In this work, a novel kind of double-stranded polyrotaxane motif was reported by Ag+-directed coordination-driven assembly following the preassembly of a four-connected pseudorotaxane (cpb)2CB8 linker. Moreover, supramolecular isomerism is observed in crystalline compounds based on double-stranded polyrotaxane motifs due to differences in lattice stacking mode. Interestingly, the resultant supramolecular isomers, cross-Ag-DSP-1 and para-Ag-DSP-1, show dual thermo- and anion-responsiveness. Benefiting from high crystallinity of these coordination assemblies, a combination of characterization techniques, especially X-ray diffraction, was used to unveil precise molecular mechanisms related to the inherent dynamic behavior of these assemblies, which can be attributed to remarkable lattice rearrangement and crystal transformations as temperature increases or after anion exchange, reflecting the adaptive adjustment ability of these supramolecular architectures in response to external stimuli. Based on the anion exchange capability, these two supramolecular materials show fast removal kinetics and high sorption capacity for perrhenate (ReO4-) anion, a surrogate of radioactive pertechnetate (TcO4-) in nuclear waste eluents. This work provides a feasible way to supramolecular assemblies with customized structures and stimuli-responsiveness, and is helpful to design and synthesize more functional supramolecular systems with complex structures and tailored functions.
2026, 37(4): 111304
doi: 10.1016/j.cclet.2025.111304
Abstract:
Alkene cross-coupling provides a simple and efficient approach for constructing C–C bonds using readily accessible alkene feedstocks. Despite significant progress in C–C bonds formation through the difunctionalization of alkenes, analogous reaction involving two distinct alkenes remains extremely limited. Herein, we report the excited-state palladium(0) catalyzed alkenylcarboxylation of two distinct alkenes with CO2, delivering a variety of carboxylic acids in moderate to excellent yields. This reaction features high regio- & chemoselectivity, broad substrate scope (> 70 examples), and facile derivatization of products. Mechanistic studies indicate that the key step for this new strategy lies in the reductive activation of electron-deficient alkenes with the excited-state palladium complex to generate alkene radical anions. The current single-electron reduction strategy for alkenes catalyzed by photoexcited palladium(0) not only broadens the scope of excited palladium chemistry but also provides a mild approach for alkenes activation. Furthermore, this method serves as an efficient tool for the rapid construction of multiple C–C bonds in a one-pot operation using two distinct alkenes.
Alkene cross-coupling provides a simple and efficient approach for constructing C–C bonds using readily accessible alkene feedstocks. Despite significant progress in C–C bonds formation through the difunctionalization of alkenes, analogous reaction involving two distinct alkenes remains extremely limited. Herein, we report the excited-state palladium(0) catalyzed alkenylcarboxylation of two distinct alkenes with CO2, delivering a variety of carboxylic acids in moderate to excellent yields. This reaction features high regio- & chemoselectivity, broad substrate scope (> 70 examples), and facile derivatization of products. Mechanistic studies indicate that the key step for this new strategy lies in the reductive activation of electron-deficient alkenes with the excited-state palladium complex to generate alkene radical anions. The current single-electron reduction strategy for alkenes catalyzed by photoexcited palladium(0) not only broadens the scope of excited palladium chemistry but also provides a mild approach for alkenes activation. Furthermore, this method serves as an efficient tool for the rapid construction of multiple C–C bonds in a one-pot operation using two distinct alkenes.
2026, 37(4): 111317
doi: 10.1016/j.cclet.2025.111317
Abstract:
Long-wavelength fluorescent dyes have revolutionized in vivo fluorescence imaging by offering unparalleled spatial resolution. Nevertheless, the majority of organic fluorescent dyes documented to date exhibit emission wavelengths predominantly within the range of 1000–1100 nm, with scarcely any surpassing the 1200 nm threshold. Herein, we introduce a heptamethine cyanine dye that boasts a remarkable fluorescence wavelength of 1239 nm. To our knowledge, this represents the longest fluorescence wavelength for heptamethine benzindole derivative. We have meticulously analyzed its photophysical characteristics and solvatochromic behavior, and assessed its efficacy in vivo fluorescence imaging applications.
Long-wavelength fluorescent dyes have revolutionized in vivo fluorescence imaging by offering unparalleled spatial resolution. Nevertheless, the majority of organic fluorescent dyes documented to date exhibit emission wavelengths predominantly within the range of 1000–1100 nm, with scarcely any surpassing the 1200 nm threshold. Herein, we introduce a heptamethine cyanine dye that boasts a remarkable fluorescence wavelength of 1239 nm. To our knowledge, this represents the longest fluorescence wavelength for heptamethine benzindole derivative. We have meticulously analyzed its photophysical characteristics and solvatochromic behavior, and assessed its efficacy in vivo fluorescence imaging applications.
2026, 37(4): 111320
doi: 10.1016/j.cclet.2025.111320
Abstract:
Bile salt hydrolase (BSH), a gatekeeper enzyme in bile acid metabolism, regulates the host's bile acid profile and is closely associated with various metabolic diseases. However, suitable methods for measuring its activity in living systems remain scarce. Herein, a novel far-red fluorogenic substrate (CA-ABEI) for BSH was designed and developed by conjugating cholic acid with an aminocoumarin fluorophore. Under physiological conditions, CA-ABEI can be rapidly hydrolyzed by BSH from various bacterial sources to form ABEI, triggering strong fluorescence enhancement at 620 nm. Specifically activated by BSH, CA-ABEI enables accurate detection of BSH activity in biospecimens, including pure enzymes, bacteria and intact fecal slurries, and the first bioimaging of BSH activity in both BSH-expressing engineered Escherichia coli and natural intestinal microbiota. Moreover, a high-throughput screening platform was established using CA-ABEI, enabling the evaluation of BSH inhibitory effects from 96 herbal extracts. Pu-erh tea emerged as a potent BSH inhibitor and its active components were subsequently characterized, aiding the discovery of novel BSH inhibitors. Collectively, CA-ABEI proved to be a powerful tool for monitoring BSH activity in complex biological systems with value for exploring physiological functions and rapid screening of inhibitors.
Bile salt hydrolase (BSH), a gatekeeper enzyme in bile acid metabolism, regulates the host's bile acid profile and is closely associated with various metabolic diseases. However, suitable methods for measuring its activity in living systems remain scarce. Herein, a novel far-red fluorogenic substrate (CA-ABEI) for BSH was designed and developed by conjugating cholic acid with an aminocoumarin fluorophore. Under physiological conditions, CA-ABEI can be rapidly hydrolyzed by BSH from various bacterial sources to form ABEI, triggering strong fluorescence enhancement at 620 nm. Specifically activated by BSH, CA-ABEI enables accurate detection of BSH activity in biospecimens, including pure enzymes, bacteria and intact fecal slurries, and the first bioimaging of BSH activity in both BSH-expressing engineered Escherichia coli and natural intestinal microbiota. Moreover, a high-throughput screening platform was established using CA-ABEI, enabling the evaluation of BSH inhibitory effects from 96 herbal extracts. Pu-erh tea emerged as a potent BSH inhibitor and its active components were subsequently characterized, aiding the discovery of novel BSH inhibitors. Collectively, CA-ABEI proved to be a powerful tool for monitoring BSH activity in complex biological systems with value for exploring physiological functions and rapid screening of inhibitors.
2026, 37(4): 111351
doi: 10.1016/j.cclet.2025.111351
Abstract:
To promote the advantages of near-infrared-Ⅱ (NIR-Ⅱ) imaging, researchers have developed various types of NIR-Ⅱ imaging contrast agents, with conjugated dyes being one of the most important categories. However, hydrophobic dyes often rely on encapsulation with amphiphilic polymers for biological applications, which lead to brightness quenching and instability in vivo. To address this, we proposed a covalent encapsulation strategy to transform the hydrophobic dye from organic solvent to aqueous solution. To achieve this, we designed a chlorine-containing NIR-Ⅱ cyanine dye (C7–1080), which covalently binds to human serum albumin (HSA), forming a stable NIR-Ⅱ fluorescent probe, HSA@C7–1080. The HSA@C7–1080 has precise molecular weight and spatial structure, making dye monodispersing in the albumin pocket with improved fluorescence and stability. This NIR-Ⅱ fluorescent probe provides high-resolution NIR-Ⅱ imaging in various biological systems. Our strategy offers a promising alternative for the clinical translation of hydrophobic NIR-Ⅱ dyes, improving their biocompatibility and imaging performance in fluorescence-guided surgery.
To promote the advantages of near-infrared-Ⅱ (NIR-Ⅱ) imaging, researchers have developed various types of NIR-Ⅱ imaging contrast agents, with conjugated dyes being one of the most important categories. However, hydrophobic dyes often rely on encapsulation with amphiphilic polymers for biological applications, which lead to brightness quenching and instability in vivo. To address this, we proposed a covalent encapsulation strategy to transform the hydrophobic dye from organic solvent to aqueous solution. To achieve this, we designed a chlorine-containing NIR-Ⅱ cyanine dye (C7–1080), which covalently binds to human serum albumin (HSA), forming a stable NIR-Ⅱ fluorescent probe, HSA@C7–1080. The HSA@C7–1080 has precise molecular weight and spatial structure, making dye monodispersing in the albumin pocket with improved fluorescence and stability. This NIR-Ⅱ fluorescent probe provides high-resolution NIR-Ⅱ imaging in various biological systems. Our strategy offers a promising alternative for the clinical translation of hydrophobic NIR-Ⅱ dyes, improving their biocompatibility and imaging performance in fluorescence-guided surgery.
2026, 37(4): 111352
doi: 10.1016/j.cclet.2025.111352
Abstract:
The cycloaddition of epoxides and CO2 has been achieved by using the designed upper-rim functionalized calix[4]arene organocatalyst in aqueous at a mild temperature under normal pressure. The upper rim of this novel calix[4]arene organocatalyst contains two hemisquaramides at the 1,4-positions. A variety of cyclic carbonate derivatives were obtained in good yields, demonstrating excellent compatibility with various functional groups. The π···π supramolecular interaction between the calixarene cavity and epoxide substrate may also play a significant role in facilitating this cycloaddition process. Additionally, this novel reaction offers a valuable complementary approach to synthesizing cyclic carbonates from epoxides and CO2.
The cycloaddition of epoxides and CO2 has been achieved by using the designed upper-rim functionalized calix[4]arene organocatalyst in aqueous at a mild temperature under normal pressure. The upper rim of this novel calix[4]arene organocatalyst contains two hemisquaramides at the 1,4-positions. A variety of cyclic carbonate derivatives were obtained in good yields, demonstrating excellent compatibility with various functional groups. The π···π supramolecular interaction between the calixarene cavity and epoxide substrate may also play a significant role in facilitating this cycloaddition process. Additionally, this novel reaction offers a valuable complementary approach to synthesizing cyclic carbonates from epoxides and CO2.
2026, 37(4): 111354
doi: 10.1016/j.cclet.2025.111354
Abstract:
Here, Friedel–Crafts (FC) reaction is used to synthesize a purely organic cage in a one-pot manner. The trigonal prismatic cage is composed of two trisfuran platforms, bridged by three phenanthrene pillars each bearing two methoxy (OMe) units. The organic cage exhibited good kinetic inertness, allowing for a synthetic post-functionalization. During this transforming process, the electron-donating methoxy (OMe) groups were converted into electron-withdrawing carbonyl groups without any degradation on the cage framework. The cage exhibits multiple guest recognition modes. The oxygen atoms as the Lewis base present in either methoxy or carbonyl before and after post-functionalization, endow the cage with the ability to recognize Lewis acidic guests such as alkali cations. The OMe and carbonyl units grated on the phenanthrene pillars endow the cage with an π-electron-rich and π-electron-deficient cavity, respectively, where π-electron-deficient and π-electron-rich guests can be accommodated.
Here, Friedel–Crafts (FC) reaction is used to synthesize a purely organic cage in a one-pot manner. The trigonal prismatic cage is composed of two trisfuran platforms, bridged by three phenanthrene pillars each bearing two methoxy (OMe) units. The organic cage exhibited good kinetic inertness, allowing for a synthetic post-functionalization. During this transforming process, the electron-donating methoxy (OMe) groups were converted into electron-withdrawing carbonyl groups without any degradation on the cage framework. The cage exhibits multiple guest recognition modes. The oxygen atoms as the Lewis base present in either methoxy or carbonyl before and after post-functionalization, endow the cage with the ability to recognize Lewis acidic guests such as alkali cations. The OMe and carbonyl units grated on the phenanthrene pillars endow the cage with an π-electron-rich and π-electron-deficient cavity, respectively, where π-electron-deficient and π-electron-rich guests can be accommodated.
2026, 37(4): 111377
doi: 10.1016/j.cclet.2025.111377
Abstract:
Polyfunctionalized axial-chiral 2-arylpyridines are important class of chiral entities in organic synthesis and drug discovery. However, practical synthesis of such structures remains underdeveloped. Herein, we report a novel synthetic method via simple cobalt-catalyzed [2 + 2 + 2] cycloaddition reactions of easily accessible diynes with nitriles. A wide range of polyfunctionalized axial-chiral 2-arylpyridine derivatives were obtained with high enantioselectivities and atom economy by using 2-methyl tetrahydrofuran (2-MeTHF) as a green solvent. Notably, the axial-chiral 2-arylpyridine N-oxide compounds and chiral bispyridine derivatives have been accessible in high efficiency using this simple protocol. The mechanism and origin of regioselectivity of this reaction was revealed using DFT calculation profiles.
Polyfunctionalized axial-chiral 2-arylpyridines are important class of chiral entities in organic synthesis and drug discovery. However, practical synthesis of such structures remains underdeveloped. Herein, we report a novel synthetic method via simple cobalt-catalyzed [2 + 2 + 2] cycloaddition reactions of easily accessible diynes with nitriles. A wide range of polyfunctionalized axial-chiral 2-arylpyridine derivatives were obtained with high enantioselectivities and atom economy by using 2-methyl tetrahydrofuran (2-MeTHF) as a green solvent. Notably, the axial-chiral 2-arylpyridine N-oxide compounds and chiral bispyridine derivatives have been accessible in high efficiency using this simple protocol. The mechanism and origin of regioselectivity of this reaction was revealed using DFT calculation profiles.
2026, 37(4): 111433
doi: 10.1016/j.cclet.2025.111433
Abstract:
Core-shell magnetic polymer microspheres with mesoporous organic shells hold immense potential in diverse applications, encompassing adsorption, separation, delivery/immobilization of guest molecules in catalysis and controlled drug release. Herein, magnetic mesoporous melamine-formaldehyde resin microspheres (Fe3O4@SiO2@mMF) are constructed via a nanoemulsion-assisted interfacial co-assembly and polymerization strategy, using Pluronic F127 as a template agent and soluble melamine-formaldehyde (MF) oligomer as the precursor. The resulting microspheres possess radially oriented mesopores, superparamagnetic properties, and abundant N-containing active sites (nitrogen content: 15.02 wt%). The as-synthesized Fe3O4@SiO2@mMF microspheres as ideal catalyst supports, exhibit exceptional loading capacity for phosphotungstic acid (PTA). The as-formed Fe3O4@SiO2@mMF/PTA composites demonstrate not only good catalytic performance in the esterification reaction of n-butanol and acetic acid with a high conversion of 92% (to acetic acid) but also excellent antimicrobial performance against Staphylococcus aureus and Escherichia coli with viabilities of 11.58% and 7.35%, respectively.
Core-shell magnetic polymer microspheres with mesoporous organic shells hold immense potential in diverse applications, encompassing adsorption, separation, delivery/immobilization of guest molecules in catalysis and controlled drug release. Herein, magnetic mesoporous melamine-formaldehyde resin microspheres (Fe3O4@SiO2@mMF) are constructed via a nanoemulsion-assisted interfacial co-assembly and polymerization strategy, using Pluronic F127 as a template agent and soluble melamine-formaldehyde (MF) oligomer as the precursor. The resulting microspheres possess radially oriented mesopores, superparamagnetic properties, and abundant N-containing active sites (nitrogen content: 15.02 wt%). The as-synthesized Fe3O4@SiO2@mMF microspheres as ideal catalyst supports, exhibit exceptional loading capacity for phosphotungstic acid (PTA). The as-formed Fe3O4@SiO2@mMF/PTA composites demonstrate not only good catalytic performance in the esterification reaction of n-butanol and acetic acid with a high conversion of 92% (to acetic acid) but also excellent antimicrobial performance against Staphylococcus aureus and Escherichia coli with viabilities of 11.58% and 7.35%, respectively.
2026, 37(4): 111453
doi: 10.1016/j.cclet.2025.111453
Abstract:
The deficiency of reliable and physiologically relevant distal lung models has been regarded as a crucial issue for drug research on non small cell lung cancer (NSCLC). In this study, an inverse opal structure-based lung-on-a-chip was established to replicate the geometric dimensions and topography of the native lung alveoli, and two lateral microchambers were designed to induce pressure-driven stretching for the simulation of respiratory movement. Further, a concentration gradient generator was applied to connect with lung-on-a-chip for the creation of different enzyme environments to mimic the individual variability of P450s enzymes in lung patients. Based on this microfluidic platform, the Osimertinib implications in NSLC was investigated from the aspect of metabolism and adapted resistance. The results suggested that Osimertinib exhibited discernible difference in metabolism under diverse enzyme condition. Additionally, in contrast with the control group, all groups with Osimertinib treatment triggered the alterations of amino acid metabolisms and energy supply, indicating that targeting energy supply process might be an effective measure to prevent tumor cells from generating drug resistance.
The deficiency of reliable and physiologically relevant distal lung models has been regarded as a crucial issue for drug research on non small cell lung cancer (NSCLC). In this study, an inverse opal structure-based lung-on-a-chip was established to replicate the geometric dimensions and topography of the native lung alveoli, and two lateral microchambers were designed to induce pressure-driven stretching for the simulation of respiratory movement. Further, a concentration gradient generator was applied to connect with lung-on-a-chip for the creation of different enzyme environments to mimic the individual variability of P450s enzymes in lung patients. Based on this microfluidic platform, the Osimertinib implications in NSLC was investigated from the aspect of metabolism and adapted resistance. The results suggested that Osimertinib exhibited discernible difference in metabolism under diverse enzyme condition. Additionally, in contrast with the control group, all groups with Osimertinib treatment triggered the alterations of amino acid metabolisms and energy supply, indicating that targeting energy supply process might be an effective measure to prevent tumor cells from generating drug resistance.
2026, 37(4): 111463
doi: 10.1016/j.cclet.2025.111463
Abstract:
Carbon nitride (CN)-based photocatalytic processes hold promise for water decontamination, during which the widely acknowledged charge transfer pathway is unfortunately characterized by severe chemical stability challenges. Herein, the intensive yet underestimated energy transfer pathway is achieved in CN nanosheets for durable, efficient, and sustainable water purification. Upon simple oxygen activation in air, the synthesized nanosheets come with an optimal pollutant removal rate constant of 0.18 min−1 under visible light irradiation, far exceeding that of state-of-the-art photocatalysts. It is revealed that the enhanced exciton binding energy inside the CN nanosheets triggers strong exciton effects, promoting the accumulation of triplet-state excitons by regulating the energy gap. The accumulated triplet excitons almost accomplish the transition from oxygen exclusively to singlet oxygen via the energy transfer pathway, which ultimately contributes to the robust degradation of the pollutants. This work proposes a viable strategy to enhance the exciton effect within CN, upon which efficient water treatment technology driven by energy transfer pathways can be expected.
Carbon nitride (CN)-based photocatalytic processes hold promise for water decontamination, during which the widely acknowledged charge transfer pathway is unfortunately characterized by severe chemical stability challenges. Herein, the intensive yet underestimated energy transfer pathway is achieved in CN nanosheets for durable, efficient, and sustainable water purification. Upon simple oxygen activation in air, the synthesized nanosheets come with an optimal pollutant removal rate constant of 0.18 min−1 under visible light irradiation, far exceeding that of state-of-the-art photocatalysts. It is revealed that the enhanced exciton binding energy inside the CN nanosheets triggers strong exciton effects, promoting the accumulation of triplet-state excitons by regulating the energy gap. The accumulated triplet excitons almost accomplish the transition from oxygen exclusively to singlet oxygen via the energy transfer pathway, which ultimately contributes to the robust degradation of the pollutants. This work proposes a viable strategy to enhance the exciton effect within CN, upon which efficient water treatment technology driven by energy transfer pathways can be expected.
2026, 37(4): 111488
doi: 10.1016/j.cclet.2025.111488
Abstract:
Cervical cancer remains a leading cause of cancer-related mortality in women, underscoring the urgent need for advanced diagnostic and therapeutic strategies. Current imaging techniques face significant limitations, including radiation exposure, high costs, and inadequate sensitivity for detecting early metastases, particularly in imaging and diagnosing tumor metastatic lesions. To overcome these challenges, we developed a multimodal imaging strategy that combined near-infrared fluorescence (NIRF, 750–1700 nm) imaging with X-ray imaging, with assistance of innovative nanomaterial to achieve precise tumor targeting and comprehensive diagnostic. Specifically, we synthesized a folate acid-functionalized polydopamine-modified ICG-Bi2Se3 nanocomposite (FA-PDA@ICG-Bi2Se3, FPBI), which integrated the complementary advantages of NIRF, X-ray, and computerized tomography imaging. The FPBI nanocomposite leveraged the targeting capability of folate acid for specific identification of cervical cancer lesions and metastatic lymph node. Furthermore, it demonstrated robust photothermal therapeutic efficacy under near-infrared (808 nm) excitation, achieving significant tumor ablation effects. This work provides an innovative nanoplatform based strategy for multimodal imaging, precise diagnosis, and targeted therapy of cervical cancer, paving the way for improved detection and management of metastatic lesions.
Cervical cancer remains a leading cause of cancer-related mortality in women, underscoring the urgent need for advanced diagnostic and therapeutic strategies. Current imaging techniques face significant limitations, including radiation exposure, high costs, and inadequate sensitivity for detecting early metastases, particularly in imaging and diagnosing tumor metastatic lesions. To overcome these challenges, we developed a multimodal imaging strategy that combined near-infrared fluorescence (NIRF, 750–1700 nm) imaging with X-ray imaging, with assistance of innovative nanomaterial to achieve precise tumor targeting and comprehensive diagnostic. Specifically, we synthesized a folate acid-functionalized polydopamine-modified ICG-Bi2Se3 nanocomposite (FA-PDA@ICG-Bi2Se3, FPBI), which integrated the complementary advantages of NIRF, X-ray, and computerized tomography imaging. The FPBI nanocomposite leveraged the targeting capability of folate acid for specific identification of cervical cancer lesions and metastatic lymph node. Furthermore, it demonstrated robust photothermal therapeutic efficacy under near-infrared (808 nm) excitation, achieving significant tumor ablation effects. This work provides an innovative nanoplatform based strategy for multimodal imaging, precise diagnosis, and targeted therapy of cervical cancer, paving the way for improved detection and management of metastatic lesions.
2026, 37(4): 111492
doi: 10.1016/j.cclet.2025.111492
Abstract:
Photovoltaic micron-silicon scrap (m-Si) has attracted attention as an anode material for lithium-ion batteries due to its high purity and low cost. However, its large particle size hinders the practical application. Herein, we propose an electrochemical etching process in molten KCl-LiCl to reduce its size. A novel electrode pair was developed by combining m-Si (anode) and spent lithium iron phosphate (LFP, cathode) material from spent lithium-ion batteries (LIBs). The m-Si was reduced from 10 µm to <5 µm at a cell voltage of 3.0 V by electrochemical etching without chlorine gas and was porous. The obtained e-Si-50 anode exhibits a high specific capacity of 1061.2 mAh/g at 2.0 A/g after 800 cycles in lithium-ion batteries. The Li3PO4, Fe, and carbon are derived by the electrochemical reduction of the LFP, and are efficiently separated via magnetic separation in water without acid/base treatment. This process combines the recycling of photovoltaic micro-silicon scrap and spent LIBs, providing both environmental and economic benefits.
Photovoltaic micron-silicon scrap (m-Si) has attracted attention as an anode material for lithium-ion batteries due to its high purity and low cost. However, its large particle size hinders the practical application. Herein, we propose an electrochemical etching process in molten KCl-LiCl to reduce its size. A novel electrode pair was developed by combining m-Si (anode) and spent lithium iron phosphate (LFP, cathode) material from spent lithium-ion batteries (LIBs). The m-Si was reduced from 10 µm to <5 µm at a cell voltage of 3.0 V by electrochemical etching without chlorine gas and was porous. The obtained e-Si-50 anode exhibits a high specific capacity of 1061.2 mAh/g at 2.0 A/g after 800 cycles in lithium-ion batteries. The Li3PO4, Fe, and carbon are derived by the electrochemical reduction of the LFP, and are efficiently separated via magnetic separation in water without acid/base treatment. This process combines the recycling of photovoltaic micro-silicon scrap and spent LIBs, providing both environmental and economic benefits.
2026, 37(4): 111516
doi: 10.1016/j.cclet.2025.111516
Abstract:
Supramolecular architectures exhibiting cascade energy transfer characteristics represent pivotal model systems for advancing biomimetic light-harvesting systems (LHS) that emulate the natural photosynthesis. To now, the engineering of aqueous-phase artificial LHS with optimized energy transfer cascades is still a challenge. In this study, we designed and synthesized two tetraphenylethylene (TPE)-based macrocyclic compounds (namely TPE-1 and TPE-2) with different cavity sizes as supramolecular scaffolds to study their energy transfer behaviors. As a control model, a linear molecule TPE-3 was also prepared. The bigger-cavity macrocycle TPE-1 can emit green fluorescence and self-assemble into nanospherical structures in aqueous media, acting as an energy donor. Through self-assembly with eosin Y (EY) and a red-emitting fluorophore (TPE-Se), a sequential Förster resonance energy transfer (FRET) cascade: TPE-1→EY→TPE-Se was achieved thanks to their excellent spectral overlap and proximity between the donor and acceptors. The optimized ternary system (TPE-1/EY/TPE-Se) with a ratio of 1000:90:60 afforded a high energy transfer efficiency (ΦET) of 95%. Then, the artificial LHS platform catalyzed the oxidative coupling of benzylamines with 93% yield in aqueous media. Moreover, the system demonstrated broad catalytic utility oxidation reactions, the good conversion of methylthiobenzyl ester to methylbenzene sulfoxide and the aerobic cross-dehydrogenation coupling reaction of N-phenyltetrahydroisoquinoline with indole. These results robustly demonstrate the promising potential of this artificial LHS in the field of aqueous photocatalysis.
Supramolecular architectures exhibiting cascade energy transfer characteristics represent pivotal model systems for advancing biomimetic light-harvesting systems (LHS) that emulate the natural photosynthesis. To now, the engineering of aqueous-phase artificial LHS with optimized energy transfer cascades is still a challenge. In this study, we designed and synthesized two tetraphenylethylene (TPE)-based macrocyclic compounds (namely TPE-1 and TPE-2) with different cavity sizes as supramolecular scaffolds to study their energy transfer behaviors. As a control model, a linear molecule TPE-3 was also prepared. The bigger-cavity macrocycle TPE-1 can emit green fluorescence and self-assemble into nanospherical structures in aqueous media, acting as an energy donor. Through self-assembly with eosin Y (EY) and a red-emitting fluorophore (TPE-Se), a sequential Förster resonance energy transfer (FRET) cascade: TPE-1→EY→TPE-Se was achieved thanks to their excellent spectral overlap and proximity between the donor and acceptors. The optimized ternary system (TPE-1/EY/TPE-Se) with a ratio of 1000:90:60 afforded a high energy transfer efficiency (ΦET) of 95%. Then, the artificial LHS platform catalyzed the oxidative coupling of benzylamines with 93% yield in aqueous media. Moreover, the system demonstrated broad catalytic utility oxidation reactions, the good conversion of methylthiobenzyl ester to methylbenzene sulfoxide and the aerobic cross-dehydrogenation coupling reaction of N-phenyltetrahydroisoquinoline with indole. These results robustly demonstrate the promising potential of this artificial LHS in the field of aqueous photocatalysis.
2026, 37(4): 111522
doi: 10.1016/j.cclet.2025.111522
Abstract:
The design of covalent organic frameworks (COFs) with strong fluorescence in both solid and solution states present a significant challenge for white-light-emitting diode (WLED) applications, primarily due to the difficulty of balancing aggregation-induced emission (AIE) and aggregation-caused quenching (ACQ). Here, we report the synthesis of a 7-fold interpenetrated three-dimensional COF (3D COF) with a pts topology, termed ZJUT-M, constructed by co-condensation of a T4-symmetric monomer with two D2h-symmetric fluorophores exhibiting distinct emission behaviors. ZJUT-M displays robust fluorescence in both solid and solution states, enabling its use in WLEDs. Mechanistic studies reveal that the dual-mode emission is driven by the synergistic integration of high-degree-of-freedom chromophores, which promote AIE emission in the solid state, and conformationally restricted fluorophores, which suppress ACQ effect in solution. These findings provide a strategic pathway for achieving multi-state emissive COFs, opening avenues for their application in advanced optoelectronic devices, including next-generation LEDs.
The design of covalent organic frameworks (COFs) with strong fluorescence in both solid and solution states present a significant challenge for white-light-emitting diode (WLED) applications, primarily due to the difficulty of balancing aggregation-induced emission (AIE) and aggregation-caused quenching (ACQ). Here, we report the synthesis of a 7-fold interpenetrated three-dimensional COF (3D COF) with a pts topology, termed ZJUT-M, constructed by co-condensation of a T4-symmetric monomer with two D2h-symmetric fluorophores exhibiting distinct emission behaviors. ZJUT-M displays robust fluorescence in both solid and solution states, enabling its use in WLEDs. Mechanistic studies reveal that the dual-mode emission is driven by the synergistic integration of high-degree-of-freedom chromophores, which promote AIE emission in the solid state, and conformationally restricted fluorophores, which suppress ACQ effect in solution. These findings provide a strategic pathway for achieving multi-state emissive COFs, opening avenues for their application in advanced optoelectronic devices, including next-generation LEDs.
2026, 37(4): 111538
doi: 10.1016/j.cclet.2025.111538
Abstract:
This study employed the ferrate(Ⅵ)/sulfur(Ⅳ) (Fe(Ⅵ)/S(Ⅳ)) system to degrade aromatic organoarsenic compounds, with a focus on elucidating the role of in situ-formed Fe(Ⅲ) flocs. The introduction of S(Ⅳ) significantly enhanced oxidative degradation efficiency compared to Fe(Ⅵ) alone, achieving 94.8% p-arsanilic acid (p-ASA) degradation within 3 min. The evolution of active species under varying S(Ⅳ) dosages was systematically investigated via radical quenching experiments and probe compound analysis. SO4•−, •OH and Fe(Ⅳ)/Fe(Ⅴ) were identified as the dominant reactive species in the Fe(Ⅵ)/S(Ⅳ) system, with Fe(Ⅳ)/Fe(Ⅴ) serving as the primary driver of p-ASA degradation. Characterization revealed that Fe(Ⅲ) flocs contributed to arsenic (As) adsorption. While S(Ⅳ) addition altered the morphology and structure of Fe(Ⅲ) flocs, these changes exerted negligible effects on As adsorption capacity. A plausible degradation pathway for p-ASA was proposed, supported by density functional theory (DFT) calculations and degradation product analysis. The system demonstrated robust resistance to common interfering ions, while the low toxicity of degradation byproducts highlighted its potential as a sustainable technology for AOCs elimination. This work elucidated structural modifications in Fe(Ⅲ) flocs induced by S(Ⅳ) and underscored the pivotal role of Fe(Ⅳ)/Fe(Ⅴ), positioning the Fe(Ⅵ)/S(Ⅳ) system as a promising strategy for AOCs degradation.
This study employed the ferrate(Ⅵ)/sulfur(Ⅳ) (Fe(Ⅵ)/S(Ⅳ)) system to degrade aromatic organoarsenic compounds, with a focus on elucidating the role of in situ-formed Fe(Ⅲ) flocs. The introduction of S(Ⅳ) significantly enhanced oxidative degradation efficiency compared to Fe(Ⅵ) alone, achieving 94.8% p-arsanilic acid (p-ASA) degradation within 3 min. The evolution of active species under varying S(Ⅳ) dosages was systematically investigated via radical quenching experiments and probe compound analysis. SO4•−, •OH and Fe(Ⅳ)/Fe(Ⅴ) were identified as the dominant reactive species in the Fe(Ⅵ)/S(Ⅳ) system, with Fe(Ⅳ)/Fe(Ⅴ) serving as the primary driver of p-ASA degradation. Characterization revealed that Fe(Ⅲ) flocs contributed to arsenic (As) adsorption. While S(Ⅳ) addition altered the morphology and structure of Fe(Ⅲ) flocs, these changes exerted negligible effects on As adsorption capacity. A plausible degradation pathway for p-ASA was proposed, supported by density functional theory (DFT) calculations and degradation product analysis. The system demonstrated robust resistance to common interfering ions, while the low toxicity of degradation byproducts highlighted its potential as a sustainable technology for AOCs elimination. This work elucidated structural modifications in Fe(Ⅲ) flocs induced by S(Ⅳ) and underscored the pivotal role of Fe(Ⅳ)/Fe(Ⅴ), positioning the Fe(Ⅵ)/S(Ⅳ) system as a promising strategy for AOCs degradation.
2026, 37(4): 111547
doi: 10.1016/j.cclet.2025.111547
Abstract:
Species at the air-water interface of microdroplets often display distinct acidity compared to the bulk. In this study, we report that pyrrole, imidazole, pyrazole, and 2H-1,2,3-triazole, a group of five-membered, planar, aromatic, nitrogen heterocyclic compounds that are basic in bulk water, exhibit strong acidity on microdroplets. The deprotonated anions of pyrrole, imidazole, and pyrazole can further react with CO2 to generate the corresponding carboxylic acids, but the triazole anion does not react with CO2. Calculation shows that partial solvation and the electric field on the air-water interface of the microdroplets are the main causes for the increased acidity, and the unique solvation structure of the triazole anion at the interface causes the reactive sites to be shielded by interfacial water molecules, thereby hindering reaction with CO2. These results demonstrate that the electric field and solvation structure of ions at the air-water interface play a decisive role in microdroplet chemistry for these compounds. We anticipate that the unique acidity and reactivity on microdroplets provide a new avenue that is rich in opportunities for green chemistry.
Species at the air-water interface of microdroplets often display distinct acidity compared to the bulk. In this study, we report that pyrrole, imidazole, pyrazole, and 2H-1,2,3-triazole, a group of five-membered, planar, aromatic, nitrogen heterocyclic compounds that are basic in bulk water, exhibit strong acidity on microdroplets. The deprotonated anions of pyrrole, imidazole, and pyrazole can further react with CO2 to generate the corresponding carboxylic acids, but the triazole anion does not react with CO2. Calculation shows that partial solvation and the electric field on the air-water interface of the microdroplets are the main causes for the increased acidity, and the unique solvation structure of the triazole anion at the interface causes the reactive sites to be shielded by interfacial water molecules, thereby hindering reaction with CO2. These results demonstrate that the electric field and solvation structure of ions at the air-water interface play a decisive role in microdroplet chemistry for these compounds. We anticipate that the unique acidity and reactivity on microdroplets provide a new avenue that is rich in opportunities for green chemistry.
2026, 37(4): 111567
doi: 10.1016/j.cclet.2025.111567
Abstract:
The development of a high-performance pH-universal electrocatalyst for hydrogen evolution reaction (HER) is a vital step toward hydrogen economy but remains a major challenge. Herein, the Pd, Cu, and Ni three elements were confined in a nanoparticle via the microemulsion method. Morphology and structural analysis reveal that PdCuNi nanoparticles are nearly spherical in shape with slight aggregation, and are mainly composed of metallic Pd and Cu, as well as Ni oxide. The electrochemical tests show that PdCuNi exhibits favorable HER catalytic activity in acid (ŋ10: 45 mV; Tafel slopes: 33 mV/dec) and neutral (ŋ10: 71 mV; Tafel slopes: 87 mV/dec) media, and alkaline (ŋ10: 66 mV; Tafel slopes: 116 mV/dec) media. The mechanism analysis implies that the synergistic effect of Pd, Cu, and Ni can improve the inherent conductivity of the catalyst and accelerate the charge transfer process. Furthermore, over 30 h long-term stability has been achieved without significant attenuation. This work provides a strategy for developing versatile and robust multimetallic catalysts towards pH-universal HER.
The development of a high-performance pH-universal electrocatalyst for hydrogen evolution reaction (HER) is a vital step toward hydrogen economy but remains a major challenge. Herein, the Pd, Cu, and Ni three elements were confined in a nanoparticle via the microemulsion method. Morphology and structural analysis reveal that PdCuNi nanoparticles are nearly spherical in shape with slight aggregation, and are mainly composed of metallic Pd and Cu, as well as Ni oxide. The electrochemical tests show that PdCuNi exhibits favorable HER catalytic activity in acid (ŋ10: 45 mV; Tafel slopes: 33 mV/dec) and neutral (ŋ10: 71 mV; Tafel slopes: 87 mV/dec) media, and alkaline (ŋ10: 66 mV; Tafel slopes: 116 mV/dec) media. The mechanism analysis implies that the synergistic effect of Pd, Cu, and Ni can improve the inherent conductivity of the catalyst and accelerate the charge transfer process. Furthermore, over 30 h long-term stability has been achieved without significant attenuation. This work provides a strategy for developing versatile and robust multimetallic catalysts towards pH-universal HER.
2026, 37(4): 111581
doi: 10.1016/j.cclet.2025.111581
Abstract:
Cocatalysts are pivotal in realizing photocatalytic overall water splitting (POWS) by mitigating carrier recombination and expediting reaction kinetics. Nevertheless, conventional cocatalysts still faces with challenges in balancing high efficiency and low cost. Herein, adjacent CoP and CoOOH, as noble-metal-free dual cocatalysts for hydrogen/oxygen evolution, are introduced onto the surface of Al-doped SrTiO3 (Al: STO), achieving stable and efficient POWS, with a hydrogen and oxygen evolution rate of 4.86 and 2.30 mmol h-1 g-1, respectively, and an apparent quantum yield of 12.7% at 350 ± 10 nm. The superior performance is attributed to the unique adjacent structure of CoP and CoOOH dual cocatalysts. Functioning as critical reactive sites for hydrogen and oxygen evolution, respectively, co-modification of CoP and CoOOH effectively promotes the surface redox reaction. Notably, due to the Schottky junction form between CoP and CoOOH, the uniformly distributed and tightly attached adjacent CoP-CoOOH dual cocatalysts shortened the distance of both charge-carrier migration from bulk to the surface of photocatalyst and proton transfer from oxidation sites to reduction sites, thereby enhancing the charge-separation efficiency and protecting CoP against oxidation during photocatalytic overall water splitting process. This work offers innovative insights for designing efficient, noble-metal-free cocatalysts for POWS.
Cocatalysts are pivotal in realizing photocatalytic overall water splitting (POWS) by mitigating carrier recombination and expediting reaction kinetics. Nevertheless, conventional cocatalysts still faces with challenges in balancing high efficiency and low cost. Herein, adjacent CoP and CoOOH, as noble-metal-free dual cocatalysts for hydrogen/oxygen evolution, are introduced onto the surface of Al-doped SrTiO3 (Al: STO), achieving stable and efficient POWS, with a hydrogen and oxygen evolution rate of 4.86 and 2.30 mmol h-1 g-1, respectively, and an apparent quantum yield of 12.7% at 350 ± 10 nm. The superior performance is attributed to the unique adjacent structure of CoP and CoOOH dual cocatalysts. Functioning as critical reactive sites for hydrogen and oxygen evolution, respectively, co-modification of CoP and CoOOH effectively promotes the surface redox reaction. Notably, due to the Schottky junction form between CoP and CoOOH, the uniformly distributed and tightly attached adjacent CoP-CoOOH dual cocatalysts shortened the distance of both charge-carrier migration from bulk to the surface of photocatalyst and proton transfer from oxidation sites to reduction sites, thereby enhancing the charge-separation efficiency and protecting CoP against oxidation during photocatalytic overall water splitting process. This work offers innovative insights for designing efficient, noble-metal-free cocatalysts for POWS.
2026, 37(4): 111619
doi: 10.1016/j.cclet.2025.111619
Abstract:
Calcium hydride (CaH2) is a hydrogen storage material with high hydrogen storage density that is easy to transport and store. However, its hydrogen generation process is intense and liquid water causes uneven reactions in CaH2. These two issues make the reaction of CaH2 hard to control. To resolve the issues, a gel/nonwoven fabric composite material was prepared using nonwoven fabric and poly(vinyl alcohol)/polyacrylamide (PVA/PAM) hydrogel, and applied to a compact hydrogen generator. Water absorption and evaporation tests on composite membranes confirm that the membrane can control the water transport rate by adjusting the gel content, thereby regulating the hydrogen production of CaH2. During the hydrolysis of CaH2, the heat released promotes water evaporation, which absorbs some of this heat and helps maintain both temperature and water balance. When the gel content was 10%, the height of the separator was 1 mm, and the mass of CaH2 was 1.5 g, the hydrogen generator achieved the fastest hydrogen production rate of 58.7 mL/min. Moreover, after expanding the size of the hydrogen generator, it can continuously produce hydrogen for over 260 min at room temperature. Finally, hydrogen was supplied to a proton exchange membrane fuel cell (PEMFC) stack. This research provides a new concept for controllable hydrogen production and portable fuel cells.
Calcium hydride (CaH2) is a hydrogen storage material with high hydrogen storage density that is easy to transport and store. However, its hydrogen generation process is intense and liquid water causes uneven reactions in CaH2. These two issues make the reaction of CaH2 hard to control. To resolve the issues, a gel/nonwoven fabric composite material was prepared using nonwoven fabric and poly(vinyl alcohol)/polyacrylamide (PVA/PAM) hydrogel, and applied to a compact hydrogen generator. Water absorption and evaporation tests on composite membranes confirm that the membrane can control the water transport rate by adjusting the gel content, thereby regulating the hydrogen production of CaH2. During the hydrolysis of CaH2, the heat released promotes water evaporation, which absorbs some of this heat and helps maintain both temperature and water balance. When the gel content was 10%, the height of the separator was 1 mm, and the mass of CaH2 was 1.5 g, the hydrogen generator achieved the fastest hydrogen production rate of 58.7 mL/min. Moreover, after expanding the size of the hydrogen generator, it can continuously produce hydrogen for over 260 min at room temperature. Finally, hydrogen was supplied to a proton exchange membrane fuel cell (PEMFC) stack. This research provides a new concept for controllable hydrogen production and portable fuel cells.
2026, 37(4): 111624
doi: 10.1016/j.cclet.2025.111624
Abstract:
Carbohydrates play essential roles in the physiological and pathological functions of cells. However, carbohydrate structures involve numerous levels of isomerism, which has posed significant challenges to advancements in glycomics. The technique for carbohydrate recognition needs to be precise in determining all aspects of the stereodiversity for both fundamental research and practical applications. Via quantum tunneling simulations and model analysis, we show that a carbon nanotube based nanopore as a molecular tweezer to trap a single target analyte with controlled dwell time achieved through reversible flexoelectric gating. Under mechanical deformation, the pore walls act as dynamic electrostatic binding sites to capture analyte enabling ample but fast sampling. After establishing Fano resonance as the sensing mechanism to quantitatively evaluate the interaction between the pore wall and analyte, random forest classifier algorithm is employed to classify the quantum transport data. This sensing strategy provides a general discrimination accuracy of higher than 99.4% for identifying carbohydrate isomers. Our findings highlight the efficacy of this combined physics and machine learning-based method in addressing the stereochemical complexity of carbohydrates. The approach not only improves observation time per molecule but also operates in a high-throughput format, offering a powerful artificial intelligence (AI)-empowered biomolecule sensing tool for glycomics research.
Carbohydrates play essential roles in the physiological and pathological functions of cells. However, carbohydrate structures involve numerous levels of isomerism, which has posed significant challenges to advancements in glycomics. The technique for carbohydrate recognition needs to be precise in determining all aspects of the stereodiversity for both fundamental research and practical applications. Via quantum tunneling simulations and model analysis, we show that a carbon nanotube based nanopore as a molecular tweezer to trap a single target analyte with controlled dwell time achieved through reversible flexoelectric gating. Under mechanical deformation, the pore walls act as dynamic electrostatic binding sites to capture analyte enabling ample but fast sampling. After establishing Fano resonance as the sensing mechanism to quantitatively evaluate the interaction between the pore wall and analyte, random forest classifier algorithm is employed to classify the quantum transport data. This sensing strategy provides a general discrimination accuracy of higher than 99.4% for identifying carbohydrate isomers. Our findings highlight the efficacy of this combined physics and machine learning-based method in addressing the stereochemical complexity of carbohydrates. The approach not only improves observation time per molecule but also operates in a high-throughput format, offering a powerful artificial intelligence (AI)-empowered biomolecule sensing tool for glycomics research.
2026, 37(4): 111626
doi: 10.1016/j.cclet.2025.111626
Abstract:
Sustainable photochemical CO2 conversion represents a promising strategy for mitigating excess CO2 emissions and achieving "carbon neutrality". The development of advanced catalysts with an abundance of active sites and efficient separation of photo-generated charge carriers remains a significant challenge. Here, we present a high-entropy (HE) photocatalyst by integrating five metals into Prussian blue (PB) to afford Kx(MnFeCoNiCu)[Fe(CN)6] (HE-PBA) which exhibits a high concentration of active centers and rapid electron transfer, enabling superior CO2-to-CO photoreduction performance. The HE-PBA composite catalyst delivered a high CO yield (up to 1220.5 µmol g-1 h-1), achieving near 100% product selectivity. A mechanistic analysis has revealed strong coupling and overlapping multi-atomic orbitals, which facilitates local electron redistribution and a readjustment of electron density. This effect serves to generate abundant reactive sites with CO2 interactions that facilitate C-O bond activation. Additionally, an efficient electron transfer driven by the disparity in metal electronegativity inhibits unwanted recombination of electron-hole pairs. More significantly, the photoelectrons migrate and accumulate on the HE-PBA surface, exhibiting extended long lifetimes and robust reduction ability. The findings of this study provide important insights that can contribute to the development of high-entropy materials rich in transition metals with far-ranging potential applications.
Sustainable photochemical CO2 conversion represents a promising strategy for mitigating excess CO2 emissions and achieving "carbon neutrality". The development of advanced catalysts with an abundance of active sites and efficient separation of photo-generated charge carriers remains a significant challenge. Here, we present a high-entropy (HE) photocatalyst by integrating five metals into Prussian blue (PB) to afford Kx(MnFeCoNiCu)[Fe(CN)6] (HE-PBA) which exhibits a high concentration of active centers and rapid electron transfer, enabling superior CO2-to-CO photoreduction performance. The HE-PBA composite catalyst delivered a high CO yield (up to 1220.5 µmol g-1 h-1), achieving near 100% product selectivity. A mechanistic analysis has revealed strong coupling and overlapping multi-atomic orbitals, which facilitates local electron redistribution and a readjustment of electron density. This effect serves to generate abundant reactive sites with CO2 interactions that facilitate C-O bond activation. Additionally, an efficient electron transfer driven by the disparity in metal electronegativity inhibits unwanted recombination of electron-hole pairs. More significantly, the photoelectrons migrate and accumulate on the HE-PBA surface, exhibiting extended long lifetimes and robust reduction ability. The findings of this study provide important insights that can contribute to the development of high-entropy materials rich in transition metals with far-ranging potential applications.
2026, 37(4): 111627
doi: 10.1016/j.cclet.2025.111627
Abstract:
Extensive research has been devoted to single-atom activation of persulfates in recent years. However, mechanistic understanding of the distinct interactions between different persulfates (i.e., peroxymonosulfate (PMS) and peroxydisulfate (PDS)) and the coordination environments of single-atom catalysts (SACs) remains critical for advancing their practical applications. Herein, we developed a Fe-N4 SAC exhibiting dual activation capabilities for both PMS and PDS. Intriguingly, experimental results revealed divergent activation mechanisms: PMS activation was predominantly mediated via single-site reactions generating singlet oxygen (1O2), whereas PDS activation proceeded through both dual-site and single-site pathways involving concurrent 1O2 generation and electron transfer processes. Density functional theory calculations further demonstrated that the geometric alignment between the inter-site distances of Fe-N4 centers and the molecular dimensions of PDS serves as the key determinant for enabling the electron transfer pathway. This fundamental structure-reactivity correlation suggests that the intrinsic molecular-scale differences between PMS and PDS govern their distinct interaction mechanisms with Fe-N4 SACs. Finally, the scale-up experiments realized nearly complete sulfamethoxazole degradation during 120 h continuous operation without obvious decline in both the Fe-N4/PMS and Fe-N4/PDS systems. This work provides fundamental insights into molecular-scale effects on persulfate activation mechanisms, establishing new design principles for SACs optimization in advanced oxidation processes.
Extensive research has been devoted to single-atom activation of persulfates in recent years. However, mechanistic understanding of the distinct interactions between different persulfates (i.e., peroxymonosulfate (PMS) and peroxydisulfate (PDS)) and the coordination environments of single-atom catalysts (SACs) remains critical for advancing their practical applications. Herein, we developed a Fe-N4 SAC exhibiting dual activation capabilities for both PMS and PDS. Intriguingly, experimental results revealed divergent activation mechanisms: PMS activation was predominantly mediated via single-site reactions generating singlet oxygen (1O2), whereas PDS activation proceeded through both dual-site and single-site pathways involving concurrent 1O2 generation and electron transfer processes. Density functional theory calculations further demonstrated that the geometric alignment between the inter-site distances of Fe-N4 centers and the molecular dimensions of PDS serves as the key determinant for enabling the electron transfer pathway. This fundamental structure-reactivity correlation suggests that the intrinsic molecular-scale differences between PMS and PDS govern their distinct interaction mechanisms with Fe-N4 SACs. Finally, the scale-up experiments realized nearly complete sulfamethoxazole degradation during 120 h continuous operation without obvious decline in both the Fe-N4/PMS and Fe-N4/PDS systems. This work provides fundamental insights into molecular-scale effects on persulfate activation mechanisms, establishing new design principles for SACs optimization in advanced oxidation processes.
2026, 37(4): 111630
doi: 10.1016/j.cclet.2025.111630
Abstract:
The Fenton-like activation of peroxymonosulfate (PMS) is an effective oxidation strategy for water decontamination, however, Fe(Ⅱ)-mediated Fenton-like reactions suffer from limitations of sluggish iron species cycling and iron sludge accumulation. Herein, molybdenum pentaboride (Mo2B5) was innovatively employed as a dual-functional co-catalyst to address these challenges via synergistically direct and indirect routes for activating PMS. Mo2B5 can promptly enhance Fe(Ⅲ)/PMS to entirely degrade sulfamethoxazole within 4 min, superior to conventional reducing agents and carbon-based co-catalysts. Based on mechanism investigations (reactive oxygen species analysis, iron species variation, surface chemistry characterizations), the distinctive electronic configuration of Mo2B5 can direct activate PMS for generating hydroxyl radical (•OH), while simultaneously enhance Fe(Ⅱ) regeneration to facilitate subsequent Fenton-like processes to produce sulfate radicals (SO4•−) and ferryl species (Fe(Ⅳ)). The system thus demonstrated broad applicability for degrading diverse pollutants with high rate constants, while the substrate specific reactivities are dependent on the electron-donating capacities of pollutants. In addition, Mo2B5 exhibits exceptional stability over consecutive cycle tests, attributed to its self-cleaning surface and retained crystallinity.
The Fenton-like activation of peroxymonosulfate (PMS) is an effective oxidation strategy for water decontamination, however, Fe(Ⅱ)-mediated Fenton-like reactions suffer from limitations of sluggish iron species cycling and iron sludge accumulation. Herein, molybdenum pentaboride (Mo2B5) was innovatively employed as a dual-functional co-catalyst to address these challenges via synergistically direct and indirect routes for activating PMS. Mo2B5 can promptly enhance Fe(Ⅲ)/PMS to entirely degrade sulfamethoxazole within 4 min, superior to conventional reducing agents and carbon-based co-catalysts. Based on mechanism investigations (reactive oxygen species analysis, iron species variation, surface chemistry characterizations), the distinctive electronic configuration of Mo2B5 can direct activate PMS for generating hydroxyl radical (•OH), while simultaneously enhance Fe(Ⅱ) regeneration to facilitate subsequent Fenton-like processes to produce sulfate radicals (SO4•−) and ferryl species (Fe(Ⅳ)). The system thus demonstrated broad applicability for degrading diverse pollutants with high rate constants, while the substrate specific reactivities are dependent on the electron-donating capacities of pollutants. In addition, Mo2B5 exhibits exceptional stability over consecutive cycle tests, attributed to its self-cleaning surface and retained crystallinity.
2026, 37(4): 111636
doi: 10.1016/j.cclet.2025.111636
Abstract:
The integration of advanced sensing materials as channel layers in devices is essential for constructing field-effect transistor (FET) biosensors. In this study, we synthesized high-crystallinity bimetallic M3(hexaaminotriphenylene)2 (M = Co, Ni) thin films as FET channel materials via an in-situ growth method using a mixed solvent system of water and N,N-dimethylformamide (DMF). This bimetallic metal-organic framework (MOF)-based FET then served as a glucose biosensor, achieving a high sensitivity and an ultra-wide detection range from 10 nmol/L to 10 mmol/L. Further studies reveal that the success of in-situ growth of the high-crystalline bimetallic MOF film can be attributed to the coordination solvent exchange reaction between the metal atomic center, DMF, and water. Furthermore, the introduction of bimetallic centers enhances the number of active sites within the MOF, thereby achieving an ultra-low detection limit and an ultra-wide detection range. This work presents a versatile approach for constructing high performance FET biosensors.
The integration of advanced sensing materials as channel layers in devices is essential for constructing field-effect transistor (FET) biosensors. In this study, we synthesized high-crystallinity bimetallic M3(hexaaminotriphenylene)2 (M = Co, Ni) thin films as FET channel materials via an in-situ growth method using a mixed solvent system of water and N,N-dimethylformamide (DMF). This bimetallic metal-organic framework (MOF)-based FET then served as a glucose biosensor, achieving a high sensitivity and an ultra-wide detection range from 10 nmol/L to 10 mmol/L. Further studies reveal that the success of in-situ growth of the high-crystalline bimetallic MOF film can be attributed to the coordination solvent exchange reaction between the metal atomic center, DMF, and water. Furthermore, the introduction of bimetallic centers enhances the number of active sites within the MOF, thereby achieving an ultra-low detection limit and an ultra-wide detection range. This work presents a versatile approach for constructing high performance FET biosensors.
2026, 37(4): 111644
doi: 10.1016/j.cclet.2025.111644
Abstract:
Elucidating the synergistic influence mechanism of catalysts composition and pollutants structure on the treatment system is a necessary way to further expand the application potential of heterogeneous iron-based Fenton-like technology in the field of water treatment from catalytic source and degradation end. In this study, a nitrogen-doped iron-carbon material (Fe-NC-4%) was synthesized to effectively activate peroxymonosulfate (PMS) to remove different organic pollutants, thus further exploring the synergistic effects of material and pollutant structures on degradation performance and mechanism. A combination of characterization analysis, experimental demonstration and density functional theory calculation showed that the more graphitic nitrogen in Fe-NC-4% assisted the Fe active centers to adsorb PMS more easily and further form the Fe-NC-4%-PMS* complex with high activity and stability. And the Fe-NC-4%-PMS* complex could efficiently and selectively degraded electron-donating organics by electron transfer process (ETP). The degradation rate of ofloxacin (OFL) with stronger electron-donating ability could reach 0.405 min−1 in the Fe-NC-4%/PMS system. In addition, the Fe-NC-4%/PMS system possessed strong environmental adaptability, safety and practical application potential. This study would provide technical and theoretical guidance for the top-down analysis of specific reaction mechanisms in Fenton-like systems, including catalyst structure design, reactive species generation and selective pollutant degradation.
Elucidating the synergistic influence mechanism of catalysts composition and pollutants structure on the treatment system is a necessary way to further expand the application potential of heterogeneous iron-based Fenton-like technology in the field of water treatment from catalytic source and degradation end. In this study, a nitrogen-doped iron-carbon material (Fe-NC-4%) was synthesized to effectively activate peroxymonosulfate (PMS) to remove different organic pollutants, thus further exploring the synergistic effects of material and pollutant structures on degradation performance and mechanism. A combination of characterization analysis, experimental demonstration and density functional theory calculation showed that the more graphitic nitrogen in Fe-NC-4% assisted the Fe active centers to adsorb PMS more easily and further form the Fe-NC-4%-PMS* complex with high activity and stability. And the Fe-NC-4%-PMS* complex could efficiently and selectively degraded electron-donating organics by electron transfer process (ETP). The degradation rate of ofloxacin (OFL) with stronger electron-donating ability could reach 0.405 min−1 in the Fe-NC-4%/PMS system. In addition, the Fe-NC-4%/PMS system possessed strong environmental adaptability, safety and practical application potential. This study would provide technical and theoretical guidance for the top-down analysis of specific reaction mechanisms in Fenton-like systems, including catalyst structure design, reactive species generation and selective pollutant degradation.
2026, 37(4): 111648
doi: 10.1016/j.cclet.2025.111648
Abstract:
Lithium–sulfur (Li–S) batteries with the high theoretical capacity of 1675 mAh/g have attracted attention as next-generation energy storage systems. Understanding the dynamic evolution and reaction mechanisms at the interface between sulfur cathodes and the electrolyte is crucial to achieve a high reversible capacity of Li−S batteries. However, due to the challenges in probing the complex Li–S redox reaction, the structural and morphological changes from active sulfur to insoluble lithium sulfide (Li2S) under operating conditions remain poorly understood. Here, the behaviors during sulfur dissolution and Li2S deposition/decomposition under realistic conditions were investigated via in situ atomic force microscopy (AFM). Direct visualizations revealed that tightly stacked sulfur particles hinder essential electronic pathways within the cathode. Furthermore constructing a conductive framework promotes more uniform Li2S deposition, which was previously dispersed across the electrode surface, thus accelerating Li2S conversion kinetics during the subsequent charge process. PeakForce tunneling atomic force microscopy (TUNA) measurements effectively elucidated the correlation between nanoscale structural features and electrical conductivity under varying potentials. Real-time observations reveal the dynamic evolution and reaction mechanisms of sulfur cathodes, offering profound insights into the Li−S redox processes and guiding the rational design of advanced cathodes.
Lithium–sulfur (Li–S) batteries with the high theoretical capacity of 1675 mAh/g have attracted attention as next-generation energy storage systems. Understanding the dynamic evolution and reaction mechanisms at the interface between sulfur cathodes and the electrolyte is crucial to achieve a high reversible capacity of Li−S batteries. However, due to the challenges in probing the complex Li–S redox reaction, the structural and morphological changes from active sulfur to insoluble lithium sulfide (Li2S) under operating conditions remain poorly understood. Here, the behaviors during sulfur dissolution and Li2S deposition/decomposition under realistic conditions were investigated via in situ atomic force microscopy (AFM). Direct visualizations revealed that tightly stacked sulfur particles hinder essential electronic pathways within the cathode. Furthermore constructing a conductive framework promotes more uniform Li2S deposition, which was previously dispersed across the electrode surface, thus accelerating Li2S conversion kinetics during the subsequent charge process. PeakForce tunneling atomic force microscopy (TUNA) measurements effectively elucidated the correlation between nanoscale structural features and electrical conductivity under varying potentials. Real-time observations reveal the dynamic evolution and reaction mechanisms of sulfur cathodes, offering profound insights into the Li−S redox processes and guiding the rational design of advanced cathodes.
2026, 37(4): 111654
doi: 10.1016/j.cclet.2025.111654
Abstract:
Flexible gas sensors show promise in wearable health monitoring and toxic gas detection due to mechanical flexibility and system integration, but they still face challenges such as slow response/recovery dynamics and poor stability. Here, a novel aqueous ink consisting of n-type mesoporous tin oxide (mSnO2) colloids and p-type poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate) (abbreviated as PEDOT:PSS) was designed and deposited on oxygen plasma treated polyimine (PI) substrate with pre-printed electrodes and heater via automatic dispension printing followed with a subsequent freeze-drying treatment, resuling in hierarchically porous sensing layer with mesopore channels and macroporous framework on the flexible PI substrate. The resultant SnO2/PEDOT:PSS sensor showed excellent sensing performance (6%-30.5%) toward low-concentration ammonia (1–100 ppm), rapid response/recovery speed (61 s/25 s) and superior mechanical stability. Furthermore, the sensor was integrated into a Bluetooth-enabled smart bracelet, achieving real-time monitoring of environmetal ammonia concentration and showcasing its potential for wearable electronics in dectecting volatile harmful gases.
Flexible gas sensors show promise in wearable health monitoring and toxic gas detection due to mechanical flexibility and system integration, but they still face challenges such as slow response/recovery dynamics and poor stability. Here, a novel aqueous ink consisting of n-type mesoporous tin oxide (mSnO2) colloids and p-type poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate) (abbreviated as PEDOT:PSS) was designed and deposited on oxygen plasma treated polyimine (PI) substrate with pre-printed electrodes and heater via automatic dispension printing followed with a subsequent freeze-drying treatment, resuling in hierarchically porous sensing layer with mesopore channels and macroporous framework on the flexible PI substrate. The resultant SnO2/PEDOT:PSS sensor showed excellent sensing performance (6%-30.5%) toward low-concentration ammonia (1–100 ppm), rapid response/recovery speed (61 s/25 s) and superior mechanical stability. Furthermore, the sensor was integrated into a Bluetooth-enabled smart bracelet, achieving real-time monitoring of environmetal ammonia concentration and showcasing its potential for wearable electronics in dectecting volatile harmful gases.
2026, 37(4): 111667
doi: 10.1016/j.cclet.2025.111667
Abstract:
The exposure of specific facets in catalysts plays a pivotal role in surface/interface reactions. This study systematically explores facet engineering as a novel approach to enhancing the piezoelectric and piezo-photocatalytic capabilities of metal-organic frameworks (MOFs), with a focus on ZIF-8 as a model compound. By selectively exposing specific facets-(100), (110), and a combination of both in mixed configurations, this research examines how facet orientation affects piezoelectric properties, charge separation efficiency, and catalytic performance. The ZIF-8 samples, identified as ZIF-8-RD, ZIF-8-CUBE, ZIF-8-TRD1, and ZIF-8-TRD2 demonstrated distinct catalytic activities in photocatalysis, piezocatalysis, and piezo-photocatalysis. Notably, ZIF-8-TRDs, with the mixed-facet exposure, showed superior catalytic performance, achieving up to 94% degradation of tetracycline (TC) in piezo-photocatalysis, a substantial improvement over the single-facet variant. This enhanced performance is attributed to the mixed facets' higher carrier concentration and superior charge separation facilitated by the increased internal piezoelectric potential. Density functional theory (DFT) calculations corroborate the experimental results, revealing that mixed facets contribute to a larger dipole moment, indicating greater structural asymmetry and piezoelectric efficiency. The findings underscore facet engineering as an effective strategy to optimize MOF-based catalysts, opening avenues for high-performance materials tailored for environmental remediation and sustainable energy applications. This work not only pioneers facet engineering in MOF piezo-photocatalysts but also opens new avenues for the development and enhancement of high-performance MOF in piezoelectricity.
The exposure of specific facets in catalysts plays a pivotal role in surface/interface reactions. This study systematically explores facet engineering as a novel approach to enhancing the piezoelectric and piezo-photocatalytic capabilities of metal-organic frameworks (MOFs), with a focus on ZIF-8 as a model compound. By selectively exposing specific facets-(100), (110), and a combination of both in mixed configurations, this research examines how facet orientation affects piezoelectric properties, charge separation efficiency, and catalytic performance. The ZIF-8 samples, identified as ZIF-8-RD, ZIF-8-CUBE, ZIF-8-TRD1, and ZIF-8-TRD2 demonstrated distinct catalytic activities in photocatalysis, piezocatalysis, and piezo-photocatalysis. Notably, ZIF-8-TRDs, with the mixed-facet exposure, showed superior catalytic performance, achieving up to 94% degradation of tetracycline (TC) in piezo-photocatalysis, a substantial improvement over the single-facet variant. This enhanced performance is attributed to the mixed facets' higher carrier concentration and superior charge separation facilitated by the increased internal piezoelectric potential. Density functional theory (DFT) calculations corroborate the experimental results, revealing that mixed facets contribute to a larger dipole moment, indicating greater structural asymmetry and piezoelectric efficiency. The findings underscore facet engineering as an effective strategy to optimize MOF-based catalysts, opening avenues for high-performance materials tailored for environmental remediation and sustainable energy applications. This work not only pioneers facet engineering in MOF piezo-photocatalysts but also opens new avenues for the development and enhancement of high-performance MOF in piezoelectricity.
2026, 37(4): 111668
doi: 10.1016/j.cclet.2025.111668
Abstract:
With the continuous detection of new pollutants in the water environment, their potential harm cannot be ignored. In order to explore an effective method to remove contaminants from wastewater, this paper presents an underwater bubble plasma (UBP) activated peroxymonosulfate (PMS) strategy for rapidly degrading the typical emerging contaminant tetracycline hydrochloride (TC) in water. The results indicate that, compared with UBP alone (41.1%), the UBP-PMS system (98.6%) exhibits significantly enhanced degradation ability, achieving a 57.5% increase in TC degradation rate under identical conditions while enabling long-term self-purification of wastewater without energy input within this system. In addition, we studied the effects of initial TC concentration, the type of working gas, the initial pH value of the solution, and the water matrix on the degradation performance of the UBP-PMS system. The anti-interference performance of the UBP-PMS system is proven to be strong, as six inorganic anions (HCO3−, CO32−, NO3−, HPO42−, SO42− and Cl−) are added respectively to simulate the actual water environment. The contribution of different reactive species to the degradation process was evaluated qualitatively and quantitatively by electron spin resonance (ESR) and scavenger experiments, of which the largest contribution was •OH, followed by 1O2, ONOOH/O2•-, SO4•‒ and hydrated electrons. The potential degradation pathways of TC were analyzed, and the toxicity of the degradation intermediates was evaluated by quantitative structure-activity relationship (QSAR) analysis, revealing a gradual reduction in TC toxicity under the co-treatment of UBP-PMS. This study provides a novel activation strategy involving UBP-PMS and provides valuable insights into the degradation properties and mechanisms of emerging pollutants in actual water bodies.
With the continuous detection of new pollutants in the water environment, their potential harm cannot be ignored. In order to explore an effective method to remove contaminants from wastewater, this paper presents an underwater bubble plasma (UBP) activated peroxymonosulfate (PMS) strategy for rapidly degrading the typical emerging contaminant tetracycline hydrochloride (TC) in water. The results indicate that, compared with UBP alone (41.1%), the UBP-PMS system (98.6%) exhibits significantly enhanced degradation ability, achieving a 57.5% increase in TC degradation rate under identical conditions while enabling long-term self-purification of wastewater without energy input within this system. In addition, we studied the effects of initial TC concentration, the type of working gas, the initial pH value of the solution, and the water matrix on the degradation performance of the UBP-PMS system. The anti-interference performance of the UBP-PMS system is proven to be strong, as six inorganic anions (HCO3−, CO32−, NO3−, HPO42−, SO42− and Cl−) are added respectively to simulate the actual water environment. The contribution of different reactive species to the degradation process was evaluated qualitatively and quantitatively by electron spin resonance (ESR) and scavenger experiments, of which the largest contribution was •OH, followed by 1O2, ONOOH/O2•-, SO4•‒ and hydrated electrons. The potential degradation pathways of TC were analyzed, and the toxicity of the degradation intermediates was evaluated by quantitative structure-activity relationship (QSAR) analysis, revealing a gradual reduction in TC toxicity under the co-treatment of UBP-PMS. This study provides a novel activation strategy involving UBP-PMS and provides valuable insights into the degradation properties and mechanisms of emerging pollutants in actual water bodies.
2026, 37(4): 111670
doi: 10.1016/j.cclet.2025.111670
Abstract:
Chemodynamic therapy (CDT) based on nanozyme has received much attention for safe and effective cancer treatment. However, the catalytic ability of nanozyme and insufficient intracellular H2O2 levels severely limit their therapeutic effect. To overcome these limitations, we construct tumor microenvironment-responsive hybrid cascade systems, where single-atom Cu nanozymes (CuNC SANs) with high peroxidase (POD)-like activity were synthesized to immobilize glucose oxidase (GOx). To enhance their biological performance and stability, polyethylene glycol (DSPE-PEG-NH2) is further modified. After endocytosis into tumor cells, the immobilized GOx of cascade systems reacts with intracellular glucose to produce H2O2 in situ. The H2O2 with elevated concentration can be further catalyzed by CuNC SANs and increase ROS yield after cascade reaction, thus amplifying the effect of CDT. In addition, the consumption of glucose cuts off the energy supply of the tumor, realizing starvation therapy. Significantly, the photothermal properties of CuNC SANs not only accelerate the cascade reaction but also enable photothermal therapy (PTT) for cancer treatment. This study proposes a promising PTT/CDT/starvation triple therapy strategy for high-efficiency cancer therapy.
Chemodynamic therapy (CDT) based on nanozyme has received much attention for safe and effective cancer treatment. However, the catalytic ability of nanozyme and insufficient intracellular H2O2 levels severely limit their therapeutic effect. To overcome these limitations, we construct tumor microenvironment-responsive hybrid cascade systems, where single-atom Cu nanozymes (CuNC SANs) with high peroxidase (POD)-like activity were synthesized to immobilize glucose oxidase (GOx). To enhance their biological performance and stability, polyethylene glycol (DSPE-PEG-NH2) is further modified. After endocytosis into tumor cells, the immobilized GOx of cascade systems reacts with intracellular glucose to produce H2O2 in situ. The H2O2 with elevated concentration can be further catalyzed by CuNC SANs and increase ROS yield after cascade reaction, thus amplifying the effect of CDT. In addition, the consumption of glucose cuts off the energy supply of the tumor, realizing starvation therapy. Significantly, the photothermal properties of CuNC SANs not only accelerate the cascade reaction but also enable photothermal therapy (PTT) for cancer treatment. This study proposes a promising PTT/CDT/starvation triple therapy strategy for high-efficiency cancer therapy.
2026, 37(4): 111674
doi: 10.1016/j.cclet.2025.111674
Abstract:
The melt-transesterification polycondensation method necessitates elevated reaction temperatures and protracted reaction times in the copolymerization of modified isosorbide-based polycarbonates. This results in a decline in molecular weight and color degradation of the copolymerized IS-PC. In this paper, the process of polyethylene glycol (PEG) modification was introduced in the synthesis of isosorbide-based copolycarbonate (PEXHDCYC) by means of a melt chain extension method. As demonstrated by experimental findings, this method has the capacity to reduce the reaction temperature and shorten the reaction time. Additionally, it has been observed to enhance the molecular weight and overall properties of the material. Through the optimization of reaction conditions, a series of PEXHDCYC with weight average molecular weight (Mw) ranging from 19,004 g/mol to 73,294 g/mol were synthesized. The results demonstrated that the glass transition temperature (Tg) of PEXHDCYC decreased in conjunction with an increase in the PEG1000 content. It is noteworthy that the PEXHDCYC synthesized by this method exhibits an exceptional elongation at break, reaching up to 135.45% ± 24%. Furthermore, PEXHDCYC demonstrates superior optical properties in comparison to bisphenol A polycarbonate (BPA-PC).
The melt-transesterification polycondensation method necessitates elevated reaction temperatures and protracted reaction times in the copolymerization of modified isosorbide-based polycarbonates. This results in a decline in molecular weight and color degradation of the copolymerized IS-PC. In this paper, the process of polyethylene glycol (PEG) modification was introduced in the synthesis of isosorbide-based copolycarbonate (PEXHDCYC) by means of a melt chain extension method. As demonstrated by experimental findings, this method has the capacity to reduce the reaction temperature and shorten the reaction time. Additionally, it has been observed to enhance the molecular weight and overall properties of the material. Through the optimization of reaction conditions, a series of PEXHDCYC with weight average molecular weight (Mw) ranging from 19,004 g/mol to 73,294 g/mol were synthesized. The results demonstrated that the glass transition temperature (Tg) of PEXHDCYC decreased in conjunction with an increase in the PEG1000 content. It is noteworthy that the PEXHDCYC synthesized by this method exhibits an exceptional elongation at break, reaching up to 135.45% ± 24%. Furthermore, PEXHDCYC demonstrates superior optical properties in comparison to bisphenol A polycarbonate (BPA-PC).
2026, 37(4): 111675
doi: 10.1016/j.cclet.2025.111675
Abstract:
The electrocatalytic reduction of carbon dioxide (CO2) into fuels holds significant promise for addressing energy and environmental challenges, albeit hindered by constraints in conversion efficiency, production rates, and electrode stability. Metal diborides are considered as promising electrocatalysts that may demonstrate superior CO2 electroreduction performance due to their distinctive electronic properties. Herein, a series of novel bulk metal diborides, encompassing transition metals from group IVB to group VIIB elements, were fabricated using a high pressure-high temperature technique, which were directly utilized as self-supporting electrodes for electrocatalytic reduction of CO2. The zirconium diboride (ZrB2) electrode stood out in metal diborides with superior electrocatalytic activity in generating carbon monoxide (CO), achieving a Faradaic efficiency of 92.2% at −2.2 V vs. Ag/Ag+ in ionic liquid-based electrolytes. Impressively, the ZrB2 electrode demonstrated stable catalysis of CO2 reduction to CO over a nearly 60-h electrolysis period. Furthermore, the ZrB2 electrode and ionic liquid-based electrolytes could synergistically catalyze the reduction of CO2 to CO. Experimental results and density functional theory calculations support the notion that exposed metal sites on the ZrB2 (001) surface could enhance *CO desorption and restrain the hydrogen evolution reaction, thereby facilitating the conversion of CO2 into CO.
The electrocatalytic reduction of carbon dioxide (CO2) into fuels holds significant promise for addressing energy and environmental challenges, albeit hindered by constraints in conversion efficiency, production rates, and electrode stability. Metal diborides are considered as promising electrocatalysts that may demonstrate superior CO2 electroreduction performance due to their distinctive electronic properties. Herein, a series of novel bulk metal diborides, encompassing transition metals from group IVB to group VIIB elements, were fabricated using a high pressure-high temperature technique, which were directly utilized as self-supporting electrodes for electrocatalytic reduction of CO2. The zirconium diboride (ZrB2) electrode stood out in metal diborides with superior electrocatalytic activity in generating carbon monoxide (CO), achieving a Faradaic efficiency of 92.2% at −2.2 V vs. Ag/Ag+ in ionic liquid-based electrolytes. Impressively, the ZrB2 electrode demonstrated stable catalysis of CO2 reduction to CO over a nearly 60-h electrolysis period. Furthermore, the ZrB2 electrode and ionic liquid-based electrolytes could synergistically catalyze the reduction of CO2 to CO. Experimental results and density functional theory calculations support the notion that exposed metal sites on the ZrB2 (001) surface could enhance *CO desorption and restrain the hydrogen evolution reaction, thereby facilitating the conversion of CO2 into CO.
2026, 37(4): 111703
doi: 10.1016/j.cclet.2025.111703
Abstract:
Hydroxyethyl starch 130/0.4 (HES130/0.4) is a macromolecular polysaccharide with polydispersity, which is widely used as a plasma expander. Full-profile bioanalysis of HES130/0.4 is required to characterize its plasma pharmacokinetics, yet current analytical technologies struggle with this task due to its complex structure and composition. To address this existing lacuna within the realm of analytical science, we propose a liquid chromatography-electrospray ionization mass spectrometry (LC-ESI-MS) methodology for the full-profile bioanalysis of HES130/0.4. Amide column separation with gradient optimization eluted polydisperse HES130/0.4 as a single symmetric peak. In-source collision-induced dissociation (IS-CID) converted the numerous precursor ions of HES130/0.4 into a limited number of characteristic fragment ions, from which m/z 597.4 was selected as the "pseudo-precursor ion" for MRM quantification. The ion transition m/z 597.4 → 435.3 was identified as the quantitative ion pair. The method demonstrated a linear calibration curve from 40 µg/mL to 4000 µg/mL, with accuracy and precision meeting acceptance criteria, confirming its reliability and reproducibility. Subsequently, the workflow was successfully applied to investigate the pharmacokinetics of HES130/0.4 in rat, revealing its large distribution volume and rapid elimination within 24 h. This work provides a straightforward approach for the full-profile quantification of HES130/0.4 in biological samples, overcoming the limitations of traditional methods in terms of poor specificity, low sensitivity and narrow linear range, and providing a reference for the in vivo full-profile bioanalysis of HES130/0.4 and other polysaccharides.
Hydroxyethyl starch 130/0.4 (HES130/0.4) is a macromolecular polysaccharide with polydispersity, which is widely used as a plasma expander. Full-profile bioanalysis of HES130/0.4 is required to characterize its plasma pharmacokinetics, yet current analytical technologies struggle with this task due to its complex structure and composition. To address this existing lacuna within the realm of analytical science, we propose a liquid chromatography-electrospray ionization mass spectrometry (LC-ESI-MS) methodology for the full-profile bioanalysis of HES130/0.4. Amide column separation with gradient optimization eluted polydisperse HES130/0.4 as a single symmetric peak. In-source collision-induced dissociation (IS-CID) converted the numerous precursor ions of HES130/0.4 into a limited number of characteristic fragment ions, from which m/z 597.4 was selected as the "pseudo-precursor ion" for MRM quantification. The ion transition m/z 597.4 → 435.3 was identified as the quantitative ion pair. The method demonstrated a linear calibration curve from 40 µg/mL to 4000 µg/mL, with accuracy and precision meeting acceptance criteria, confirming its reliability and reproducibility. Subsequently, the workflow was successfully applied to investigate the pharmacokinetics of HES130/0.4 in rat, revealing its large distribution volume and rapid elimination within 24 h. This work provides a straightforward approach for the full-profile quantification of HES130/0.4 in biological samples, overcoming the limitations of traditional methods in terms of poor specificity, low sensitivity and narrow linear range, and providing a reference for the in vivo full-profile bioanalysis of HES130/0.4 and other polysaccharides.
2026, 37(4): 111704
doi: 10.1016/j.cclet.2025.111704
Abstract:
Foodborne bacterial infection is a serious threat to food safety, especially live pathogens causing outbreaks of most diseases. Thus developing live bacterial detection methods is important for public health. In this study, a microfluidic biosensor was developed for rapid detection of live Salmonella typhimurium, in which immune magnetic particle chains in microchannels were used to separate and enrich target bacteria, antibody-conjugated gold nanorods (GNRs) were applied for photothermal lysis of target live bacteria under near-infrared (NIR) irradiation, and a photon-counting detector was used for measuring adenosine triphosphate (ATP) bioluminescence in the presence of firefly luciferin/luciferase. This biosensor was proved to be able to quantitatively detect S. typhimurium from 5.0 × 102 CFU/mL to 5.0 × 106 CFU/mL in 60 min (magnetic separation 20 min; GNRs combination 20 min; NIR irradiation, 8 min) with limit of detection (LOD) of 495 CFU/mL. This biosensor showed an excellent specificity in the coexistence of other foodborne bacteria, and target bacteria were successfully measured even in the matrix interference of milk sample with mean recovery of 121.17%. This biosensor might be a promising tool for on-site assessment foodborne bacteria.
Foodborne bacterial infection is a serious threat to food safety, especially live pathogens causing outbreaks of most diseases. Thus developing live bacterial detection methods is important for public health. In this study, a microfluidic biosensor was developed for rapid detection of live Salmonella typhimurium, in which immune magnetic particle chains in microchannels were used to separate and enrich target bacteria, antibody-conjugated gold nanorods (GNRs) were applied for photothermal lysis of target live bacteria under near-infrared (NIR) irradiation, and a photon-counting detector was used for measuring adenosine triphosphate (ATP) bioluminescence in the presence of firefly luciferin/luciferase. This biosensor was proved to be able to quantitatively detect S. typhimurium from 5.0 × 102 CFU/mL to 5.0 × 106 CFU/mL in 60 min (magnetic separation 20 min; GNRs combination 20 min; NIR irradiation, 8 min) with limit of detection (LOD) of 495 CFU/mL. This biosensor showed an excellent specificity in the coexistence of other foodborne bacteria, and target bacteria were successfully measured even in the matrix interference of milk sample with mean recovery of 121.17%. This biosensor might be a promising tool for on-site assessment foodborne bacteria.
2026, 37(4): 111705
doi: 10.1016/j.cclet.2025.111705
Abstract:
E. coli O157:H7 and Staphylococcus aureus have emerged as significant foodborne pathogens, characterized by considerable incidence rates and mortality. Despite advancements, current detection methods are hindered by challenges in enhancing specificity and sensitivity. Herein, we introduced a cutting-edge biosensor that employs a novel CHA-coupled CRISPR multi-stage signal amplification technique for the rapid and ultra-sensitive detection of these two pathogens. This microfluidic device consisted of an upstream serpentine mixing channel and a downstream boat-shaped microcavity equipped with a micro-column array, facilitating efficient reagent mixing, robust CHA amplification, and CRISPR reactions. Multiple signal amplification was achieved through bacterial competitive binding triggered by catalytic hairpin assembly (CHA) and crRNA-mediated CRISPR reactions. Based on this platform, the detection of target bacteria is transformed into nucleic acid detection, with a maximum detection range of 134 CFU/mL for E. coli O157:H7 and 181 CFU/mL for Staphylococcus aureus, which were better or comparable to previously reported biosensors. The entire assay was completed within approximately 1.5 h, with a minimal sample volume requirement of just 10 µL. The biosensor exhibited a high recovery rate, ranging from 95% to 115%, and demonstrated excellent specificity towards the target bacteria. In summary, this biosensor offers a rapid, accurate, and highly sensitive tool for food safety and clinical diagnostics.
E. coli O157:H7 and Staphylococcus aureus have emerged as significant foodborne pathogens, characterized by considerable incidence rates and mortality. Despite advancements, current detection methods are hindered by challenges in enhancing specificity and sensitivity. Herein, we introduced a cutting-edge biosensor that employs a novel CHA-coupled CRISPR multi-stage signal amplification technique for the rapid and ultra-sensitive detection of these two pathogens. This microfluidic device consisted of an upstream serpentine mixing channel and a downstream boat-shaped microcavity equipped with a micro-column array, facilitating efficient reagent mixing, robust CHA amplification, and CRISPR reactions. Multiple signal amplification was achieved through bacterial competitive binding triggered by catalytic hairpin assembly (CHA) and crRNA-mediated CRISPR reactions. Based on this platform, the detection of target bacteria is transformed into nucleic acid detection, with a maximum detection range of 134 CFU/mL for E. coli O157:H7 and 181 CFU/mL for Staphylococcus aureus, which were better or comparable to previously reported biosensors. The entire assay was completed within approximately 1.5 h, with a minimal sample volume requirement of just 10 µL. The biosensor exhibited a high recovery rate, ranging from 95% to 115%, and demonstrated excellent specificity towards the target bacteria. In summary, this biosensor offers a rapid, accurate, and highly sensitive tool for food safety and clinical diagnostics.
2026, 37(4): 111708
doi: 10.1016/j.cclet.2025.111708
Abstract:
Dielectric barrier discharge (DBD) plasma combined with Fe2+ for periodate (PI) activation was proposed for emerging contaminants treatment. The feasible, activation mechanism, degradation mechanism were comprehensively analyzed. Results showed that within 6 min treatment time, the degradation efficiency of sulfadiazine (SDZ) could reach 68.1%, 78.5% and 90.2% in DBD, DBD/PI and DBD/PI/Fe2+, respectively. The energy efficiency can also be improved from 47.24 mg/kWh (DBD) to 78.43 mg/kWh (DBD/PI/Fe2+). Compared with DBD system, the PI activation energy barrier in DBD/Fe2+ system is significantly decreased. Electron spin resonance (ESR) proved the existence of •OH, 1O2 and •O2− in DBD/PI/Fe2+ system, and the corresponding intensity are higher than that of DBD/PI system. The quenching experiments shown that •OH, 1O2, •O2− and electron play important role for SDZ degradation. Reactive species dominant to SDZ degradation was explored by LC–MS and density functional theory (DFT) analysis. Higher input power, acid condition and higher conductivity were favorable to SDZ degradation. DBD/PI/Fe2+ system has good effect in treating other emerging contaminants and obtains good environmental adaptability.
Dielectric barrier discharge (DBD) plasma combined with Fe2+ for periodate (PI) activation was proposed for emerging contaminants treatment. The feasible, activation mechanism, degradation mechanism were comprehensively analyzed. Results showed that within 6 min treatment time, the degradation efficiency of sulfadiazine (SDZ) could reach 68.1%, 78.5% and 90.2% in DBD, DBD/PI and DBD/PI/Fe2+, respectively. The energy efficiency can also be improved from 47.24 mg/kWh (DBD) to 78.43 mg/kWh (DBD/PI/Fe2+). Compared with DBD system, the PI activation energy barrier in DBD/Fe2+ system is significantly decreased. Electron spin resonance (ESR) proved the existence of •OH, 1O2 and •O2− in DBD/PI/Fe2+ system, and the corresponding intensity are higher than that of DBD/PI system. The quenching experiments shown that •OH, 1O2, •O2− and electron play important role for SDZ degradation. Reactive species dominant to SDZ degradation was explored by LC–MS and density functional theory (DFT) analysis. Higher input power, acid condition and higher conductivity were favorable to SDZ degradation. DBD/PI/Fe2+ system has good effect in treating other emerging contaminants and obtains good environmental adaptability.
2026, 37(4): 111729
doi: 10.1016/j.cclet.2025.111729
Abstract:
NH4V4O10 has attracted significant attention as a cathode material for aqueous zinc-ion batteries (AZIBs) due to its adjustable interlayer spacing (~9.5 Å) and high theoretical specific capacity (~400 mAh/g). However, its development is hindered by sluggish Zn2+ kinetics and structural instability. In this work, a glycine (Gly) intercalation strategy is demonstrated, which establishes three stabilization mechanisms in the Gly-NVO cathode: (1) Gly pillars are shown to expand the interlayer spacing to 1.21 nm; (2) Hydrogen-bonding networks are formed between layers; (3) Reversible NH4+ (de)intercalation behavior is observed. The Gly-NVO cathode delivers a capacity of 520 mAh/g at 0.2 A/g (393 Wh/kg energy density), along with outstanding rate capability (400 and 150 mAh/g at 10 and 50 A/g, corresponding to power densities of 5688 and 24.3 kW/kg, respectively). A capacity retention of 88.2% is maintained after 10,000 cycles at 50 A/g. DFT calculations confirm that the introduction of Gly significantly enhances the electrical conductivity of NVO while effectively weakening electrostatic interactions, and energy barrier for Zn2+ intercalation and vanadium dissolution are reduced by Gly. Additionally, due to the reversible NH4+ (de)intercalation behavior in Gly-NVO, the assembled aqueous ammonium-ion batteries (AAIBs) exhibit stable cycling ability. This work highlights organic molecule pre-intercalation as a viable strategy for optimizing the durability of ammonium vanadate cathodes.
NH4V4O10 has attracted significant attention as a cathode material for aqueous zinc-ion batteries (AZIBs) due to its adjustable interlayer spacing (~9.5 Å) and high theoretical specific capacity (~400 mAh/g). However, its development is hindered by sluggish Zn2+ kinetics and structural instability. In this work, a glycine (Gly) intercalation strategy is demonstrated, which establishes three stabilization mechanisms in the Gly-NVO cathode: (1) Gly pillars are shown to expand the interlayer spacing to 1.21 nm; (2) Hydrogen-bonding networks are formed between layers; (3) Reversible NH4+ (de)intercalation behavior is observed. The Gly-NVO cathode delivers a capacity of 520 mAh/g at 0.2 A/g (393 Wh/kg energy density), along with outstanding rate capability (400 and 150 mAh/g at 10 and 50 A/g, corresponding to power densities of 5688 and 24.3 kW/kg, respectively). A capacity retention of 88.2% is maintained after 10,000 cycles at 50 A/g. DFT calculations confirm that the introduction of Gly significantly enhances the electrical conductivity of NVO while effectively weakening electrostatic interactions, and energy barrier for Zn2+ intercalation and vanadium dissolution are reduced by Gly. Additionally, due to the reversible NH4+ (de)intercalation behavior in Gly-NVO, the assembled aqueous ammonium-ion batteries (AAIBs) exhibit stable cycling ability. This work highlights organic molecule pre-intercalation as a viable strategy for optimizing the durability of ammonium vanadate cathodes.
2026, 37(4): 111732
doi: 10.1016/j.cclet.2025.111732
Abstract:
Materials with blue-shifted and enhanced emission exhibit extensive applications in information encryption, solar ultraviolet sensing and ink-free printing, however, preparing blue-shifted and enhanced emission from photo-responsive material remains a significant challenge. Herein, we designed and synthesized successfully the photo-responsive ionic-bonded organic crystals (IOC) using tetraphenylethylene (TPE)-based multidentate imidazolium salt and sulfonic acid. Impressively, the discernible response of IOC to UV light is evidenced by a blue shift and an enhancement in dilute solution. Specifically, this has resulted in a significant increase in the absolute quantum yield, from 7.0% to 41.3%. This remarkable efficiency can be attributed to the cooperative effect that reduces non-radiative processes, the restriction of intermolecular motions (RIM) and the modulation of charge transfer (CT) behavior. This work first reports blue-shifted and enhanced emission from ionic crystal, providing a new strategy to achieve photochromic materials.
Materials with blue-shifted and enhanced emission exhibit extensive applications in information encryption, solar ultraviolet sensing and ink-free printing, however, preparing blue-shifted and enhanced emission from photo-responsive material remains a significant challenge. Herein, we designed and synthesized successfully the photo-responsive ionic-bonded organic crystals (IOC) using tetraphenylethylene (TPE)-based multidentate imidazolium salt and sulfonic acid. Impressively, the discernible response of IOC to UV light is evidenced by a blue shift and an enhancement in dilute solution. Specifically, this has resulted in a significant increase in the absolute quantum yield, from 7.0% to 41.3%. This remarkable efficiency can be attributed to the cooperative effect that reduces non-radiative processes, the restriction of intermolecular motions (RIM) and the modulation of charge transfer (CT) behavior. This work first reports blue-shifted and enhanced emission from ionic crystal, providing a new strategy to achieve photochromic materials.
2026, 37(4): 111743
doi: 10.1016/j.cclet.2025.111743
Abstract:
Piezocatalysis offers an efficient approach for producing H2O2, a sustainable fuel and oxidant with a wide range of applications. Natural tourmaline, known for its exceptional piezoelectric properties, stands out as a promising green catalyst compared to other synthetic catalysts. In this study, natural tourmaline was modified using a simple acid treatment to remove iron, achieving effective piezocatalytic H2O2 synthesis at a rate of 513.7 µmol g−1 h−1 under ambient conditions. In-depth studies demonstrated that the Fe-free tourmaline exhibited a stronger polarization electric field due to the enhanced polyhedron distortion, compared to the Fe-containing tourmaline. The influence of temperature on their piezoresponse was also investigated. This study provides new insights into the mechanisms of piezoelectric H2O2 production using natural tourmaline.
Piezocatalysis offers an efficient approach for producing H2O2, a sustainable fuel and oxidant with a wide range of applications. Natural tourmaline, known for its exceptional piezoelectric properties, stands out as a promising green catalyst compared to other synthetic catalysts. In this study, natural tourmaline was modified using a simple acid treatment to remove iron, achieving effective piezocatalytic H2O2 synthesis at a rate of 513.7 µmol g−1 h−1 under ambient conditions. In-depth studies demonstrated that the Fe-free tourmaline exhibited a stronger polarization electric field due to the enhanced polyhedron distortion, compared to the Fe-containing tourmaline. The influence of temperature on their piezoresponse was also investigated. This study provides new insights into the mechanisms of piezoelectric H2O2 production using natural tourmaline.
2026, 37(4): 111754
doi: 10.1016/j.cclet.2025.111754
Abstract:
Hydrogel electrolyte have attracted widely interest for aqueous zinc-ion batteries because of their multi-functionality and intrinsic safety. However, the unstable anode/electrolyte interface by dendrite and side reaction (HER) restricted the cycling of Zn anode, especially at high utilization. Herein, we propose an interface engineering strategy by introducing dimethylformamide (DMF) to polyacrylamide (PAM) electrolyte which could construct the polymer-inorganic bilayer solid electrolyte interphase (SEI) to improve the interface stability and compatibility. Internal Zn5(OH)6(CO3)2 provided high modulus to suppress the dendrite physically and external polymer exhibited flexibility to accommodate the volume change of Zn during cycles. Meanwhile, larger polymer clusters were induced by enhanced hydrogen-bond interactions, resulted in higher shear strength and interfacial adhesion. Additionally, DMF regulated the crystal orientation along (100) crystal plane and solvation structure of Zn2+ with PAM, enabling dense deposition and reduced by-products. Consequently, the Zn anode could provide an impressive lifespan (0.5 mA/cm2@0.5 mAh/cm2, 4000 h; 30 mA/cm2@15 mAh/cm2, 650 h). More importantly, high utilization (68%) was achieved using ultra-thin Zn (10 µm) with superior stability (2 mA/cm2@4 mAh/cm2, 1200 h). Coupled with iodine cathode, the Zn-I2 cell could provide an initial capacity of 184.5 mAh/g at the low ratio of anode/cathode capacity (N/P: 4.3) and ~86.4% retention over 500 cycles. This work provides a promising approach to construct robust interface by hydrogel electrolyte towards practical zinc-ion batteries.
Hydrogel electrolyte have attracted widely interest for aqueous zinc-ion batteries because of their multi-functionality and intrinsic safety. However, the unstable anode/electrolyte interface by dendrite and side reaction (HER) restricted the cycling of Zn anode, especially at high utilization. Herein, we propose an interface engineering strategy by introducing dimethylformamide (DMF) to polyacrylamide (PAM) electrolyte which could construct the polymer-inorganic bilayer solid electrolyte interphase (SEI) to improve the interface stability and compatibility. Internal Zn5(OH)6(CO3)2 provided high modulus to suppress the dendrite physically and external polymer exhibited flexibility to accommodate the volume change of Zn during cycles. Meanwhile, larger polymer clusters were induced by enhanced hydrogen-bond interactions, resulted in higher shear strength and interfacial adhesion. Additionally, DMF regulated the crystal orientation along (100) crystal plane and solvation structure of Zn2+ with PAM, enabling dense deposition and reduced by-products. Consequently, the Zn anode could provide an impressive lifespan (0.5 mA/cm2@0.5 mAh/cm2, 4000 h; 30 mA/cm2@15 mAh/cm2, 650 h). More importantly, high utilization (68%) was achieved using ultra-thin Zn (10 µm) with superior stability (2 mA/cm2@4 mAh/cm2, 1200 h). Coupled with iodine cathode, the Zn-I2 cell could provide an initial capacity of 184.5 mAh/g at the low ratio of anode/cathode capacity (N/P: 4.3) and ~86.4% retention over 500 cycles. This work provides a promising approach to construct robust interface by hydrogel electrolyte towards practical zinc-ion batteries.
2026, 37(4): 111776
doi: 10.1016/j.cclet.2025.111776
Abstract:
The first example of heterogeneous direct benzylation of N-heterocycles (quinoxalin-2(1H)-ones and quinoxalines) with benzaldehydes has been accomplished via the sequence of a NaDT-photocatalyzed HAT, a single electron transfer reduction and a proton transfer, a spin-center shift and a back-HAT. Utilizing this strategy, a diverse array of benzylated N-heterocycles (29 examples) can be produced with high yields. Importantly, the DT-photocatalyzed direct benzylation with benzaldehydes would be a useful complement to the more extensively studied DT-photocatalyzed acylation and hydroxyalkylation, expanding the scope of DT photocatalysis.
The first example of heterogeneous direct benzylation of N-heterocycles (quinoxalin-2(1H)-ones and quinoxalines) with benzaldehydes has been accomplished via the sequence of a NaDT-photocatalyzed HAT, a single electron transfer reduction and a proton transfer, a spin-center shift and a back-HAT. Utilizing this strategy, a diverse array of benzylated N-heterocycles (29 examples) can be produced with high yields. Importantly, the DT-photocatalyzed direct benzylation with benzaldehydes would be a useful complement to the more extensively studied DT-photocatalyzed acylation and hydroxyalkylation, expanding the scope of DT photocatalysis.
2026, 37(4): 111781
doi: 10.1016/j.cclet.2025.111781
Abstract:
Thermo-photocatalytic CO2 conversion to C2 products exhibits high research value and industrial potential. Enhancing the catalyst's adsorption activation for CO2 and H2O, along with multistep proton-coupled electron transfer (PCET) and C-C coupling, is crucial for achieving thermo-photocatalytic CO2 reduction conversion to C2 products with H2O as a proton source in a continuous process. In this paper, we explore a novel approach utilizing biochar to obtain catalysts with more defects and combine reducing biochar with MOF Materials (ZIF-67) to get a composite (ZIF-67/PC) with substantial CO2 and H2O adsorption activation capabilities and electron density gradients. Compared to PC and ZIF-67, the ZIF-67/PC exhibited excellent catalytic performance, particularly in obtaining a certain amount of C2 products (yield 5.59 µmol g-1 h-1, selectivity 55.96%). We also investigated the structure-function relationship of the catalyst and the contributions of thermal and light effects to the catalytic reaction, aiming to guide the establishment of efficient, high-throughput catalytic CO2 conversion technologies.
Thermo-photocatalytic CO2 conversion to C2 products exhibits high research value and industrial potential. Enhancing the catalyst's adsorption activation for CO2 and H2O, along with multistep proton-coupled electron transfer (PCET) and C-C coupling, is crucial for achieving thermo-photocatalytic CO2 reduction conversion to C2 products with H2O as a proton source in a continuous process. In this paper, we explore a novel approach utilizing biochar to obtain catalysts with more defects and combine reducing biochar with MOF Materials (ZIF-67) to get a composite (ZIF-67/PC) with substantial CO2 and H2O adsorption activation capabilities and electron density gradients. Compared to PC and ZIF-67, the ZIF-67/PC exhibited excellent catalytic performance, particularly in obtaining a certain amount of C2 products (yield 5.59 µmol g-1 h-1, selectivity 55.96%). We also investigated the structure-function relationship of the catalyst and the contributions of thermal and light effects to the catalytic reaction, aiming to guide the establishment of efficient, high-throughput catalytic CO2 conversion technologies.
2026, 37(4): 111788
doi: 10.1016/j.cclet.2025.111788
Abstract:
Digital microfluidics (DMF) shows great promise in addressing the need for miniaturization and automation in immunoassay detection. Despite recent advances, an automatically operated, multiplexed heterogeneous immunoassay platform powered by DMF remains underdeveloped. Here we present a DMF platform for automated and multiplexed heterogeneous immunoassay detection by coupling spatial barcoding with automatic and uniform droplet dispensing. FluoroPel was selected as a robust hydrophobic reagent for coating the DMF top plate, and it also served as the substrate for the immuno-reaction. Its mechanical robustness was further enhanced with a Cytop CTL-809A adhesive layer under the top hydrophobic layer. Hourglass-shaped electrode patterns ensured consistent and uniform distribution of immunoassay reagents, with volume variation down to 1.0%. The analysis duration was significantly reduced from 75 min to 20 min after a heating module was integrated to elevate the immuno-reaction temperature to 37 °C. Utilizing a compact instrument featuring a multi-droplet manipulation protocol, we successfully implemented fully operated, multi-sample, multiplexed immunoassays using recombinant proteins on cell culture supernatants on the DMF platform. This innovative platform significantly enhances the efficiency, reliability, and degree of automation of DMF-actuated multiplexed heterogeneous immunoassays, potentially providing a viable solution for field deployment and multi-sample parallel diagnosis.
Digital microfluidics (DMF) shows great promise in addressing the need for miniaturization and automation in immunoassay detection. Despite recent advances, an automatically operated, multiplexed heterogeneous immunoassay platform powered by DMF remains underdeveloped. Here we present a DMF platform for automated and multiplexed heterogeneous immunoassay detection by coupling spatial barcoding with automatic and uniform droplet dispensing. FluoroPel was selected as a robust hydrophobic reagent for coating the DMF top plate, and it also served as the substrate for the immuno-reaction. Its mechanical robustness was further enhanced with a Cytop CTL-809A adhesive layer under the top hydrophobic layer. Hourglass-shaped electrode patterns ensured consistent and uniform distribution of immunoassay reagents, with volume variation down to 1.0%. The analysis duration was significantly reduced from 75 min to 20 min after a heating module was integrated to elevate the immuno-reaction temperature to 37 °C. Utilizing a compact instrument featuring a multi-droplet manipulation protocol, we successfully implemented fully operated, multi-sample, multiplexed immunoassays using recombinant proteins on cell culture supernatants on the DMF platform. This innovative platform significantly enhances the efficiency, reliability, and degree of automation of DMF-actuated multiplexed heterogeneous immunoassays, potentially providing a viable solution for field deployment and multi-sample parallel diagnosis.
2026, 37(4): 111805
doi: 10.1016/j.cclet.2025.111805
Abstract:
The extensive use of various antibiotics and organic dyes has led to increasingly severe environmental issues and posed a significant threat to human health. Developing an efficient and safe dual-functional photocatalytic material for degradation and antibacterial purposes is the key to solving environmental pollution problems. Polythiophene and covalent organic frameworks (COFs) possess excellent photophysical properties, high stability, and ease of modification, offering broad application prospects and significant development potential in the removal of organic pollutants and antibiotic-resistant bacteria (ARB). A high-performance conductive polymer PTET-T-COOH (PThC) was prepared via the Stille coupling reaction, and a bipyridine (Bpy) covalent organic framework Bpy-COF was synthesized through acid-catalyzed imine condensation. By utilizing the π-π stacking and hydrogen bonding interactions between Bpy-COF and PThC, a novel Bpy-COF/PThC all-organic heterojunction was successfully fabricated. Compared to Bpy-COF and PThC, the composite exhibits a broadened spectral response range and higher carrier separation efficiency. The 30% Bpy-COF/PThC demonstrates the best photocatalytic performance, achieving a 99.96% inactivation rate of methicillin-resistant Staphylococcus aureus (MRSA) with a cell density of 7.23 log and a 95.28% bactericidal rate of Escherichia coli (E. coli) with a cell density of 7.50 log within 60 min. Under natural light, it not only exhibits good inactivation effects on both MRSA and E. coli, but also shows excellent degradation performance for rhodamine B, methylene blue, and tetracycline. The cytotoxicity experiment demonstrates that the composite exhibits good biocompatibility and potential for practical applications. The research results provide new design ideas for constructing efficient and safe organic photocatalysts, and offer a theoretical basis for the treatment of water pollution.
The extensive use of various antibiotics and organic dyes has led to increasingly severe environmental issues and posed a significant threat to human health. Developing an efficient and safe dual-functional photocatalytic material for degradation and antibacterial purposes is the key to solving environmental pollution problems. Polythiophene and covalent organic frameworks (COFs) possess excellent photophysical properties, high stability, and ease of modification, offering broad application prospects and significant development potential in the removal of organic pollutants and antibiotic-resistant bacteria (ARB). A high-performance conductive polymer PTET-T-COOH (PThC) was prepared via the Stille coupling reaction, and a bipyridine (Bpy) covalent organic framework Bpy-COF was synthesized through acid-catalyzed imine condensation. By utilizing the π-π stacking and hydrogen bonding interactions between Bpy-COF and PThC, a novel Bpy-COF/PThC all-organic heterojunction was successfully fabricated. Compared to Bpy-COF and PThC, the composite exhibits a broadened spectral response range and higher carrier separation efficiency. The 30% Bpy-COF/PThC demonstrates the best photocatalytic performance, achieving a 99.96% inactivation rate of methicillin-resistant Staphylococcus aureus (MRSA) with a cell density of 7.23 log and a 95.28% bactericidal rate of Escherichia coli (E. coli) with a cell density of 7.50 log within 60 min. Under natural light, it not only exhibits good inactivation effects on both MRSA and E. coli, but also shows excellent degradation performance for rhodamine B, methylene blue, and tetracycline. The cytotoxicity experiment demonstrates that the composite exhibits good biocompatibility and potential for practical applications. The research results provide new design ideas for constructing efficient and safe organic photocatalysts, and offer a theoretical basis for the treatment of water pollution.
2026, 37(4): 111881
doi: 10.1016/j.cclet.2025.111881
Abstract:
Quinone-based electrode materials hold significant promise for next-generation sodium-ion batteries due to their structurally tailorable frameworks, high theoretical capacities, and favorable redox potentials. However, dissolution in organic electrolytes and structural instability during cycling critically impair their capacity retention and cycling durability. Herein, we designed and synthesized two novel acylimide materials N,N'-bis(2,6-anthraquinone diamine)-biphenyl diimide (DQ-BDI) and N,N'-bis(anthraquinone-2,6-diamine)-perylenyl diimide (DQ-PDI) with the gradual enhancement of π-conjugation. Electrochemical characterization reveals exceptional performance in DQ-PDI. At the current density of 50 mA/g, the DQ-PDI delivered the first discharge specific capacity of 158 mAh/g, and the capacity retention of 99% after 100 cycles, with the coulombic efficiency of nearly 100%. At a high current density of 500 mA/g, the DQ-PDI displays a high discharge capacity of 152 mAh/g. The reduction peaks of DQ-PDI located at 2.28 V and 1.34 V are the insertion reactions of sodium ion from the carbonyl groups on PTCDA unit and on DAAQ unit at both ends, respectively, and the two oxidation peaks at 2.58 V and 1.53 V corresponds to extraction reactions. Compared with DQ-BDI, DQ-PDI exhibits a larger π-conjugation plane, which significantly enhances the intermolecular π-π interactions. It can well reduce the dissolution of the material in organic electrolyte, resulting in a higher discharge capacity, superior cycling stability and accelerated reaction kinetics. Our π-conjugation extension strategy establishes a new paradigm for designing dissolution-resistant, high-performance organic electrodes.
Quinone-based electrode materials hold significant promise for next-generation sodium-ion batteries due to their structurally tailorable frameworks, high theoretical capacities, and favorable redox potentials. However, dissolution in organic electrolytes and structural instability during cycling critically impair their capacity retention and cycling durability. Herein, we designed and synthesized two novel acylimide materials N,N'-bis(2,6-anthraquinone diamine)-biphenyl diimide (DQ-BDI) and N,N'-bis(anthraquinone-2,6-diamine)-perylenyl diimide (DQ-PDI) with the gradual enhancement of π-conjugation. Electrochemical characterization reveals exceptional performance in DQ-PDI. At the current density of 50 mA/g, the DQ-PDI delivered the first discharge specific capacity of 158 mAh/g, and the capacity retention of 99% after 100 cycles, with the coulombic efficiency of nearly 100%. At a high current density of 500 mA/g, the DQ-PDI displays a high discharge capacity of 152 mAh/g. The reduction peaks of DQ-PDI located at 2.28 V and 1.34 V are the insertion reactions of sodium ion from the carbonyl groups on PTCDA unit and on DAAQ unit at both ends, respectively, and the two oxidation peaks at 2.58 V and 1.53 V corresponds to extraction reactions. Compared with DQ-BDI, DQ-PDI exhibits a larger π-conjugation plane, which significantly enhances the intermolecular π-π interactions. It can well reduce the dissolution of the material in organic electrolyte, resulting in a higher discharge capacity, superior cycling stability and accelerated reaction kinetics. Our π-conjugation extension strategy establishes a new paradigm for designing dissolution-resistant, high-performance organic electrodes.
2026, 37(4): 111899
doi: 10.1016/j.cclet.2025.111899
Abstract:
The stability of cathode catalyst layers (CCLs) in proton exchange membrane fuel cells (PEMFCs) is critically undermined by Pt dissolution and the loss of effective gas-water management associated with carbon support corrosion. In this work, we develop a porous TiN nanotube−supported Pt (i.e., Pt/TiN NTs) CCL that integrates robust Pt–Ti interfacial bonding with a highly accessible nanotube network to address these persistent challenges. The formation of abundant Pt–Ti bonds at the interface markedly strengthens Pt anchoring, resulting in a 2.3−fold reduction in Pt dissolution and minimal particle coarsening after accelerated durability testing compared to nanoflows-based controls dominated by Pt–N−Ti interactions. The membrane electrode assembly fabricated with this CCL achieves a peak power density of 0.81 W/cm2 and demonstrates exceptional durability, retaining 77% of its initial mass activity and 87.3% of its power density following aggressive square-wave potential cycling, meeting the 2025 U.S. Department of Energy benchmarks. Computational fluid dynamics simulation further reveal that the unique porous architecture facilitates efficient oxygen transport and rapid water removal, sustaining high catalytic utilization under operational conditions. This strategy establishes TiN NTs scaffolds as a generalizable solution for the next generation of carbon-free, high-stability catalyst layers, offering practical guidance for durable and efficient fuel cell design.
The stability of cathode catalyst layers (CCLs) in proton exchange membrane fuel cells (PEMFCs) is critically undermined by Pt dissolution and the loss of effective gas-water management associated with carbon support corrosion. In this work, we develop a porous TiN nanotube−supported Pt (i.e., Pt/TiN NTs) CCL that integrates robust Pt–Ti interfacial bonding with a highly accessible nanotube network to address these persistent challenges. The formation of abundant Pt–Ti bonds at the interface markedly strengthens Pt anchoring, resulting in a 2.3−fold reduction in Pt dissolution and minimal particle coarsening after accelerated durability testing compared to nanoflows-based controls dominated by Pt–N−Ti interactions. The membrane electrode assembly fabricated with this CCL achieves a peak power density of 0.81 W/cm2 and demonstrates exceptional durability, retaining 77% of its initial mass activity and 87.3% of its power density following aggressive square-wave potential cycling, meeting the 2025 U.S. Department of Energy benchmarks. Computational fluid dynamics simulation further reveal that the unique porous architecture facilitates efficient oxygen transport and rapid water removal, sustaining high catalytic utilization under operational conditions. This strategy establishes TiN NTs scaffolds as a generalizable solution for the next generation of carbon-free, high-stability catalyst layers, offering practical guidance for durable and efficient fuel cell design.
2026, 37(4): 111901
doi: 10.1016/j.cclet.2025.111901
Abstract:
The management of breast cancer remains clinically intractable, driven by its highly invasive behavior and limited susceptibility to conventional treatments. In this study, we engineered an innovative cyclodextrin-porphyrin co-assembled nanoplatform (CT NPs) to enable multimodal breast cancer therapy. By successfully encapsulating camptothecin (CPT) within this nanocarrier, the system (CTC NPs) achieved synergistic chemo-phototherapeutic efficacy through dual-modality action. The highly biocompatible cyclodextrin carrier significantly improved the physicochemical characteristics of CPT. In vivo studies revealed that CTC NPs effectively evaded clearance by the reticuloendothelial system, overcame the defect of premature drug leakage, and exhibited superior tumor targeting and infiltration capabilities. Under near-infrared (NIR) laser irradiation, CTC NPs can simultaneously induce localized hyperthermia and produce reactive oxygen species (ROS), thereby achieving efficient tumor ablation. In 4T1 tumor-bearing mice, CTC NPs exhibited targeted, safe, and highly potent anti-tumor efficacy, significantly suppressing both primary tumor progression (tumor suppression rate > 95%) and metastatic dissemination. In summary, this integrated nanoplatform establishes a novel theranostic paradigm for synergistic chemo-phototherapy against triple-negative breast cancer (TNBC), achieving precise tumor ablation through NIR-triggered drug release and real-time imaging guidance.
The management of breast cancer remains clinically intractable, driven by its highly invasive behavior and limited susceptibility to conventional treatments. In this study, we engineered an innovative cyclodextrin-porphyrin co-assembled nanoplatform (CT NPs) to enable multimodal breast cancer therapy. By successfully encapsulating camptothecin (CPT) within this nanocarrier, the system (CTC NPs) achieved synergistic chemo-phototherapeutic efficacy through dual-modality action. The highly biocompatible cyclodextrin carrier significantly improved the physicochemical characteristics of CPT. In vivo studies revealed that CTC NPs effectively evaded clearance by the reticuloendothelial system, overcame the defect of premature drug leakage, and exhibited superior tumor targeting and infiltration capabilities. Under near-infrared (NIR) laser irradiation, CTC NPs can simultaneously induce localized hyperthermia and produce reactive oxygen species (ROS), thereby achieving efficient tumor ablation. In 4T1 tumor-bearing mice, CTC NPs exhibited targeted, safe, and highly potent anti-tumor efficacy, significantly suppressing both primary tumor progression (tumor suppression rate > 95%) and metastatic dissemination. In summary, this integrated nanoplatform establishes a novel theranostic paradigm for synergistic chemo-phototherapy against triple-negative breast cancer (TNBC), achieving precise tumor ablation through NIR-triggered drug release and real-time imaging guidance.
2026, 37(4): 111938
doi: 10.1016/j.cclet.2025.111938
Abstract:
Two pairs of potent analgesic alkaloid enantiomers with unprecedented chemical architectures, named pyrethalkalines A (1) and B (2), were isolated from the roots of Anacyclus pyrethrum. Pyrethalkaline A (1) is an unprecedented 6/6/6/6/5-fused pentacyclic triamino alkaloid featuring a unique 8,15-diaza-pentacyclo[12.3.1.11,9.05,19.010,14]nonadecane core, and pyrethalkaline B (2) is a novel 6/6/6/6/5/6-fused hexacyclic triamino alkaloid possessing an unprecedented 8,13,19-triazahexacyclo[16.3.1.11,9.05,23.010,18.011,16]tricosane motif. Their structures were elucidated by comprehensive spectroscopic data analysis, quantum 13C nuclear magnetic resonance (NMR) DP4+ and electronic circular dichroism (ECD) calculations, and single-crystal X-ray diffraction analysis, and their plausible biosynthetic pathways were proposed. Alkaloids (±)-1 and (−)-1 at three lower doses of 1, 0.2, and 0.04 mg/kg, and (+)-2 at two lower doses of 1 and 0.2 mg/kg showed more potent analgesic activity than the positive control morphine. Further investigation revealed that (+)-1 and (−)-1 are dual transient receptor potential melastatin 8 (TRPM8) (half-maximal inhibitory concentration (IC50) = 1.90 ± 0.09 and 1.40 ± 0.17 µmol/L, respectively) and Kv1.2 inhibitors. Molecular dockings of 1 provide a novel structural model to develop potent analgesics dual targeting TRPM8 and Kv1.2 ion channels, and (±)-1 have the potential for the development of a non-opioid potent analgesic to treat neurogenic pains.
Two pairs of potent analgesic alkaloid enantiomers with unprecedented chemical architectures, named pyrethalkalines A (1) and B (2), were isolated from the roots of Anacyclus pyrethrum. Pyrethalkaline A (1) is an unprecedented 6/6/6/6/5-fused pentacyclic triamino alkaloid featuring a unique 8,15-diaza-pentacyclo[12.3.1.11,9.05,19.010,14]nonadecane core, and pyrethalkaline B (2) is a novel 6/6/6/6/5/6-fused hexacyclic triamino alkaloid possessing an unprecedented 8,13,19-triazahexacyclo[16.3.1.11,9.05,23.010,18.011,16]tricosane motif. Their structures were elucidated by comprehensive spectroscopic data analysis, quantum 13C nuclear magnetic resonance (NMR) DP4+ and electronic circular dichroism (ECD) calculations, and single-crystal X-ray diffraction analysis, and their plausible biosynthetic pathways were proposed. Alkaloids (±)-1 and (−)-1 at three lower doses of 1, 0.2, and 0.04 mg/kg, and (+)-2 at two lower doses of 1 and 0.2 mg/kg showed more potent analgesic activity than the positive control morphine. Further investigation revealed that (+)-1 and (−)-1 are dual transient receptor potential melastatin 8 (TRPM8) (half-maximal inhibitory concentration (IC50) = 1.90 ± 0.09 and 1.40 ± 0.17 µmol/L, respectively) and Kv1.2 inhibitors. Molecular dockings of 1 provide a novel structural model to develop potent analgesics dual targeting TRPM8 and Kv1.2 ion channels, and (±)-1 have the potential for the development of a non-opioid potent analgesic to treat neurogenic pains.
2026, 37(4): 112002
doi: 10.1016/j.cclet.2025.112002
Abstract:
Organic fluorescence-phosphorescence dual-emitting materials based on tunable single chromophores have attracted much attention for their broad application prospects in information technology, display media and other fields due to their high luminescence stability, simple preparation process and excellent reproducibility. Herein, we constructed a novel LP-activated fluorescence-phosphorescence dual-light-harvesting (FPRET) supramolecular assembly based on LP with orthogonal charges, the phosphorescent molecule G and the NIR dye NIB through a supramolecular non-covalent strategy. The energy transfer efficiency of fluorescence is 54.68% when the molar ratio of G/LP to NIB is 10:1, while the energy transfer efficiency and antenna effect of phosphorescence are 48.75% and 241.43 respectively when the molar ratio of G/LP to NIB is 50:1. In addition, by co-assembling with carbon dots (CDs) and adjusting the ratio of donor to acceptor components, the full-color spectral regulation including white light (CIE chromaticity coordinates x, y = 0.31, 0.33) was realized. Utilizing this LP to promote the supramolecular full-color FPRET assembly of single fluorophore G and showing the multi-level anti-counterfeiting of intelligent logic gates through pattern, time, and color editing, it provides a new insight and direction for the development of a new generation of high-performance optical functional materials.
Organic fluorescence-phosphorescence dual-emitting materials based on tunable single chromophores have attracted much attention for their broad application prospects in information technology, display media and other fields due to their high luminescence stability, simple preparation process and excellent reproducibility. Herein, we constructed a novel LP-activated fluorescence-phosphorescence dual-light-harvesting (FPRET) supramolecular assembly based on LP with orthogonal charges, the phosphorescent molecule G and the NIR dye NIB through a supramolecular non-covalent strategy. The energy transfer efficiency of fluorescence is 54.68% when the molar ratio of G/LP to NIB is 10:1, while the energy transfer efficiency and antenna effect of phosphorescence are 48.75% and 241.43 respectively when the molar ratio of G/LP to NIB is 50:1. In addition, by co-assembling with carbon dots (CDs) and adjusting the ratio of donor to acceptor components, the full-color spectral regulation including white light (CIE chromaticity coordinates x, y = 0.31, 0.33) was realized. Utilizing this LP to promote the supramolecular full-color FPRET assembly of single fluorophore G and showing the multi-level anti-counterfeiting of intelligent logic gates through pattern, time, and color editing, it provides a new insight and direction for the development of a new generation of high-performance optical functional materials.
2026, 37(4): 112096
doi: 10.1016/j.cclet.2025.112096
Abstract:
The development of efficient and cost-effective non-precious-metal single-atom catalysts (SACs) is crucial for advancing the practical application of electrocatalytic CO2 reduction (CO2RR). However, identifying highly active metal atoms and designing catalysts with uniform active center structures remain significant challenges. To address this, we developed a generic pyrolysis method to synthesize a series of transition metal-based SACs with atomically dispersed metal anchored on carbon nitride support (M-C3N4, M = Fe, Ni, Cu). Benefiting from the unique electronic structure of the Fe-N4 sites supported on C3N4, the Fe-C3N4 catalyst demonstrated exceptional performance, achieving a CO Faradaic efficiency of 99.6% and maintaining excellent stability. Theoretical calculations indicate that the Fe site exhibits a relatively stronger interaction with the *COOH intermediate, thereby helping to lower the energy barrier of the CO2 protonation process. This study provides valuable theoretical insights and practical synthesis strategies for designing high-performance non-precious-metal SACs for CO2RR.
The development of efficient and cost-effective non-precious-metal single-atom catalysts (SACs) is crucial for advancing the practical application of electrocatalytic CO2 reduction (CO2RR). However, identifying highly active metal atoms and designing catalysts with uniform active center structures remain significant challenges. To address this, we developed a generic pyrolysis method to synthesize a series of transition metal-based SACs with atomically dispersed metal anchored on carbon nitride support (M-C3N4, M = Fe, Ni, Cu). Benefiting from the unique electronic structure of the Fe-N4 sites supported on C3N4, the Fe-C3N4 catalyst demonstrated exceptional performance, achieving a CO Faradaic efficiency of 99.6% and maintaining excellent stability. Theoretical calculations indicate that the Fe site exhibits a relatively stronger interaction with the *COOH intermediate, thereby helping to lower the energy barrier of the CO2 protonation process. This study provides valuable theoretical insights and practical synthesis strategies for designing high-performance non-precious-metal SACs for CO2RR.
2026, 37(4): 112324
doi: 10.1016/j.cclet.2025.112324
Abstract:
Cancer persists as a major global health challenge, marked by high recurrence rates in aggressive malignancies such as melanoma. While immunotherapy has emerged as a promising approach, its clinical benefits are often limited by tumor immune escape mechanisms and an immunosuppressive tumor microenvironment (TME). These hurdles have driven the exploration of integrated approaches, with photothermal-immunotherapy gaining significant traction. In this study, we developed a multifunctional nanoadjuvant (MICN@PI) engineered with an acid-responsive calcium carbonate core, a hypoxia-alleviating MnO2 component, a polydopamine shell for photothermal ablation, and co-loaded immunomodulators (imiquimod and indoximod). The MnO2 in the nanoadjuvant catalytically converted the overexpressed H2O2 in the TME into O2. Concurrently, the combined action of imiquimod and indoximod orchestrated a potent adaptive immune response. Upon near-infrared laser irradiation, MICN@PI achieved significant tumor ablation, inhibited recurrence, and prolonged survival in a murine melanoma model, offering a safe and effective synergistic photothermal-immunotherapy strategy for cancer treatment.
Cancer persists as a major global health challenge, marked by high recurrence rates in aggressive malignancies such as melanoma. While immunotherapy has emerged as a promising approach, its clinical benefits are often limited by tumor immune escape mechanisms and an immunosuppressive tumor microenvironment (TME). These hurdles have driven the exploration of integrated approaches, with photothermal-immunotherapy gaining significant traction. In this study, we developed a multifunctional nanoadjuvant (MICN@PI) engineered with an acid-responsive calcium carbonate core, a hypoxia-alleviating MnO2 component, a polydopamine shell for photothermal ablation, and co-loaded immunomodulators (imiquimod and indoximod). The MnO2 in the nanoadjuvant catalytically converted the overexpressed H2O2 in the TME into O2. Concurrently, the combined action of imiquimod and indoximod orchestrated a potent adaptive immune response. Upon near-infrared laser irradiation, MICN@PI achieved significant tumor ablation, inhibited recurrence, and prolonged survival in a murine melanoma model, offering a safe and effective synergistic photothermal-immunotherapy strategy for cancer treatment.
2026, 37(4): 112163
doi: 10.1016/j.cclet.2025.112163
Abstract:
