硫空位提升2D/2D In2.77S4/CuInS2 S型异质结光催化还原CO2为C2H4选择性

引用本文: 崔依琳, 李中付, 张维坤, 高禹, 董志超, 刘从华. 硫空位提升2D/2D In_2.77S₄/CuInS₂ S型异质结光催化还原CO₂为C₂H₄选择性[J]. 物理化学学报, 2026, 42(7): 100274. doi: 10.1016/j.actphy.2026.100274 shu

Citation: Yilin Cui, Zhongfu Li, Weikun Zhang, Yu Gao, Zhichao Dong, Conghua Liu. Sulfur vacancies boosting C₂H₄ selectivity of 2D/2D In_2.77S₄/CuInS₂ S-scheme heterojunction for CO₂ photoreduction[J]. Acta Physico-Chimica Sinica, 2026, 42(7): 100274. doi: 10.1016/j.actphy.2026.100274 shu

硫空位提升2D/2D In_2.77S₄/CuInS₂ S型异质结光催化还原CO₂为C₂H₄选择性

1.
山东理工大学材料科学与工程学院, 山东淄博 255000;
2.
山东高校稀土催化新材料工程技术研究中心(CREC), 山东淄博 255000;
3.
高温功能陶瓷材料学科与技术中心, 山东淄博 255000;
4.
宜宾学院数学与物理学院, 四川宜宾 644000

通讯作者: 李中付,E-mail:lzf1632008@126.com; 董志超,E-mail:zc339580@126.com; 刘从华,E-mail:lch4138@163.com

基金项目:
本研究得到国家自然科学基金(22302114)、山东省自然科学基金(ZR2023QB210)、淄博市重点研发计划(校城融合)项目(2021SNPT0042)、湖南省环境光催化应用技术重点实验室开放课题(2114506)的资助。

摘要: 由于碳碳耦合动力学迟缓和多电子过程复杂，通过人工光合作用将二氧化碳转化为多碳烃仍具挑战性。本研究采用一步水热法合成了具有丰富硫空位(S_V)的超薄In_2.77S₄/CuInS₂异质结。通过原位X射线光电子能谱(XPS)、飞秒瞬态吸收光谱(fs-TAS)和光电化学表征，证实了由内建电场驱动的S型电荷转移机制。该S型异质结不仅提高了光生载流子的分离效率，同时保持了优异的还原能力，实现了二氧化碳光还原生成C₂烃类。实验数据与密度泛函理论(DFT)计算表明，硫空位缩短了铜-铟活性位点距离，优化了局部电荷密度，并降低了关键二聚体(^*CHOCO)形成的能垒，从而加速了碳碳耦合动力学。最终，In_2.77S₄/CuInS₂-4催化剂展现出优异的C₂H₄产率(47.2 μmol g^-1 h^-1)和选择性(99.1%)，这归因于S型异质结的高效载流子调控与硫空位促进的碳碳耦合动力学的协同效应。同位素标记实验进一步证实二氧化碳是该反应的唯一碳源。总体而言，这种"硫空位-异质结"策略为二氧化碳光还原制乙烯提供了优异的电子选择性，为二氧化碳资源化利用开辟了新视角。

关键词:

English

Sulfur vacancies boosting C₂H₄ selectivity of 2D/2D In_2.77S₄/CuInS₂ S-scheme heterojunction for CO₂ photoreduction

1.
School of Materials Science and Engineering, Shandong University of Technology, Zibo 255000, Shandong Province, China;
2.
Shandong Collegial Engineering Research Center of Novel Rare Earth Catalysis Materials (CREC), Zibo 255000, Shandong Province, China;
3.
Discipline and Technology Center for High Temperature Functional Ceramics, Zibo 255000, Shandong Province, China;
4.
School of Mathematics and Physics, Yibin University, Yibin 644000, Sichuan Province, China

Corresponding author: Zhongfu Li, ; Zhichao Dong, ; Conghua Liu,

Received Date: 30 January 2026
Accepted Date: 01 March 2026
Revised Date: 28 February 2026

Abstract: Converting CO₂ into multi-carbon hydrocarbons through artificial photosynthesis remains challenging due to sluggish C-C coupling dynamics and complex multi-electron processes. In this study, ultrathin In_2.77S₄/CuInS₂ heterojunctions with abundant sulfur vacancies (S_V) were synthesized via a one-step hydrothermal method. The S-scheme charge-transfer mechanism, driven by the built-in electric field, was confirmed through in situ X-ray photoelectron spectroscopy (XPS), femtosecond transient absorption spectroscopy (fs-TAS) and photoelectrochemical characterization. This S-scheme heterojunction not only enhanced the separation efficiency of photogenerated charge carriers but also maintained excellent reduction capability, enabling CO₂ photoreduction to C₂ hydrocarbons. Furthermore, experimental results and density functional theory (DFT) calculations demonstrated that S_V shortened the Cu-In active site distance, optimized the local charge density and lowered the energy barrier for critical dimer formation (*CHOCO), thereby accelerating the C-C coupling kinetics. Finally, the In_2.77S₄/CuInS₂-4 catalyst exhibited excellent yield (47.2 μmol g^-1 h^-1) and selectivity (99.1%) of C₂H₄, which attributed to the synergistic effect of efficient carrier rectification by the S scheme heterojunction and optimized C-C coupling dynamics facilitated by SV. Furthermore, isotope labeling confirmed CO₂ as the sole carbon source for the reaction. Overall, this “sulfur vacancy-heterojunction” strategy for CO₂ photoreduction to C₂H₄ with superior electron selectivity offers valuable insights into CO₂ utilization.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

硫空位提升2D/2D In_2.77S₄/CuInS₂ S型异质结光催化还原CO₂为C₂H₄选择性

通讯作者: 李中付,E-mail:lzf1632008@126.com; 董志超,E-mail:zc339580@126.com; 刘从华,E-mail:lch4138@163.com

English

Sulfur vacancies boosting C₂H₄ selectivity of 2D/2D In_2.77S₄/CuInS₂ S-scheme heterojunction for CO₂ photoreduction

Corresponding author: Zhongfu Li, ; Zhichao Dong, ; Conghua Liu,

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