废塑料促进S型NiCr2O4/孪晶Cd0.5Zn0.5S同质异质结光催化产氢

引用本文: 田静卓, 官朝红, 胡浩斌, 刘恩周, 杨东元. 废塑料促进S型NiCr₂O₄/孪晶Cd_0.5Zn_0.5S同质异质结光催化产氢[J]. 物理化学学报, 2025, 41(6): 100068. doi: 10.1016/j.actphy.2025.100068 shu

Citation: Jingzhuo Tian, Chaohong Guan, Haobin Hu, Enzhou Liu, Dongyuan Yang. Waste plastics promoted photocatalytic H₂ evolution over S-scheme NiCr₂O₄/twinned-Cd_0.5Zn_0.5S homo-heterojunction[J]. Acta Physico-Chimica Sinica, 2025, 41(6): 100068. doi: 10.1016/j.actphy.2025.100068 shu

废塑料促进S型NiCr₂O₄/孪晶Cd_0.5Zn_0.5S同质异质结光催化产氢

1.
西北大学化工学院/西安特种能源材料重点实验室, 陕西西安 710127;
2.
陕西省碳中和技术重点实验室, 陕西西安 710069;
3.
上海交通大学密西根学院, 上海 200240;
4.
陇东学院, 甘肃省陇东油气资源高效利用重点实验室, 甘肃庆阳 745000;
5.
西安科技大学化学与化工学院, 陕西西安 710054
基金项目:
中央引导地方科技发展资金项目(24ZYQM001),国家自然科学基金(22378326,11974276,22078261),陕西省自然科学基础研究计划(2023-JC-YB-115),陕西重点科技创新团队项目(2022TD-33),西北大学优秀博士学位论文培养计划(YB2024012),中国国家留学基金委员会项目(202406970056)资助

摘要: 同时提升体相和表面电荷分离与利用效率对于实现高效光催化析氢反应至关重要。本研究采用溶剂蒸发策略，将NiCr₂O₄纳米片负载于孪晶Cd_0.5Zn_0.5S (T-CZS)纳米颗粒表面，成功制备了NiCr₂O₄/T-CZS复合材料。经过优化，6% NiCr₂O₄/T-CZS在以聚乳酸(PLA)塑料为牺牲剂的NaOH溶液中析氢速率(r_H₂)达到81.4 mmol·h^-1·g^-1，这一显著提升主要归因于T-CZS由纤锌矿Cd_0.5Zn_0.5S (WZ-CZS)和闪锌矿Cd_0.5Zn_0.5S (ZB-CZS)组成，二者能带结构存在微小差异，使得WZ-CZS与ZB-CZS之间及T-CZS与NiCr₂O₄之间形成了S型电荷转移路径，从而促进了体相和界面电荷快速分离，确保了具有强还原能力的电子参与析氢反应(HER)。此外，借助NiCr₂O₄的局域表面等离子体共振(LSPR)效应，增强了体系对紫外-可见-近红外光的吸收，产生的热电子进一步促进了HER。同时，NaOH溶液增强了空穴的氧化反应驱动力，间接提高了HER动力学。研究还发现，其它金属铬酸盐(MCr_xO_y)，如CoCr₂O₄、AgCrO₂、Bi₆CrO₁₂、BaCrO₄、ZnCr₂O₄、CdCr₂O₄、CuCr₂O₄等，也能不同程度提高T-CZS析氢活性。上述研究结果表明，同质异质结中体相与界面S型电荷转移路径能够实现高效光催化产氢与废塑料降解过程的有效协同，为解决能源与环境挑战提供了新的思路。

关键词:

English

Waste plastics promoted photocatalytic H₂ evolution over S-scheme NiCr₂O₄/twinned-Cd_0.5Zn_0.5S homo-heterojunction

1.
School of Chemical Engineering/Xi'an Key Laboratory of Special Energy Materials, Northwest University, Xi'an 710127, Shaanxi Province, China;
2.
Shaanxi Key Laboratory for Carbon Neutral Technology, Xi'an 710069, Shaanxi Province, China;
3.
University of Michigan-Shanghai Jiao Tong University Joint Institute, Shanghai Jiao Tong University, Shanghai 200240, China;
4.
Gansu Key Laboratory of Efficient Utilization of Oil and Gas Resources in Longdong, Longdong University, Qingyang 745000, Gansu Province, China;
5.
School of Chemistry and Chemical Engineering, Xi'an University of Science and Technology, Xi'an 710054, Shaanxi Province, China
Received Date: 15 January 2025
Accepted Date: 18 February 2025
Revised Date: 16 February 2025
Fund Project:
The project was supported by the Local Science and Development Fund Project Guided by the Central Government (24ZYQM001), the National Natural Science Foundation of China (22378326, 11974276, 22078261), the Natural Science Basic Research Program of Shaanxi Province (2023-JC-YB-115), the Shaanxi Key Science and Technology Innovation Team Project (2022TD-33), the Excellent Doctoral Dissertation Cultivation Program at Northwestern University (YB2024012), and the Program of China Scholarship Council (202406970056).

Abstract: The simultaneous enhancement of separation and utilization of bulk and surface charges is crucial for achieving efficient photocatalytic H₂ evolution reactions. In this study, NiCr₂O₄/T-CZS composites were fabricated by incorporating NiCr₂O₄ nanosheets onto the surface of twinned Cd_0.5Zn_0.5S (T-CZS) nanoparticles using a solvent evaporation strategy. After optimization, the 6% NiCr₂O₄/T-CZS exhibited an impressive hydrogen (H₂) evolution rate (r_H₂) of 81.4 mmol·h^-1·g^-1 when employing polylactic acid (PLA) plastic as a sacrificial agent in NaOH solution. The reason behind this can be mainly attributed to the fact that T-CZS consists of wurtzite Cd_0.5Zn_0.5S (WZ-CZS) and zinc blende Cd_0.5Zn_0.5S (ZB-CZS) with slight band structure differences, thereby facilitating rapid bulk phase and interface charge separation due to the S-scheme charge transfer routes between WZ-CZS and ZB-CZS, as well as T-CZS and NiCr₂O₄. Moreover, this system can effectively retain electrons with strong reducing ability for efficient H₂ evolution reaction (HER) and generate hot electrons through the localized surface plasmon resonance (LSPR) effect of NiCr₂O₄, which enhances the absorption of UV-Vis-NIR light energy, thereby facilitating the HER process. What’s more, NaOH solution can indirectly promote the HER kinetics by enhancing the oxidative driving force of holes. Additionally, other metal chromates (MCr_xO_y), such as CoCr₂O₄, AgCrO₂, Bi₆CrO₁₂, BaCrO₄, ZnCr₂O₄, CdCr₂O₄, CuCr₂O₄ etc., were employed to enhance the activity of T-CZS too. The results show that above homo-heterojunction composites can integrate waste plastic degradation and photocatalytic H₂ evolution effectively based on their S-scheme bulk phase and interface charge separation mechanisms. This work provides new insights into energy and environmental challenges.

Key words:

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