物理化学学报 >> 2025, Vol. 41 >> Issue (11): 100142.doi: 10.1016/j.actphy.2025.100142

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促进电荷分离和增强O2吸附双重策略提升金修饰含硫空位CdIn2S4的光催化产H2O2性能

赵艳艳1,*(), 吴珍1, 张勇2, 朱必成3, 张建军3,*()   

  1. 1 商洛学院生物医药与食品工程学院, 陕西 商洛 726000
    2 湖北理工学院先进材料与绿色化工学院, 湖北 黄石 435003
    3 中国地质大学(武汉)材料与化学学院太阳能燃料实验室, 湖北 武汉 430078
  • 收稿日期:2025-06-30 修回日期:2025-07-28 录用日期:2025-07-29 发布日期:2025-09-29
  • 通讯作者: Email: zhaoyanyan41@163.com (赵艳艳)zhangjianjun@cug.edu.cn (张建军)
  • 基金资助:
    国家自然科学基金(22409128); 国家自然科学基金(22378103)

Enhancing photocatalytic H2O2 production via dual optimization of charge separation and O2 adsorption in Au-decorated S-vacancy-rich CdIn2S4

Yanyan Zhao1,*(), Zhen Wu1, Yong Zhang2, Bicheng Zhu3, Jianjun Zhang3,*()   

  1. 1 College of Biology Pharmacy and Food Engineering, Shangluo University, Shangluo 726000, Shaanxi Province, China
    2 School of Advanced Materials and Green Chemical Engineering, Hubei Polytechnic University, Huangshi 435003, Hubei Province, China
    3 Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China
  • Received:2025-06-30 Revised:2025-07-28 Accepted:2025-07-29 Published:2025-09-29
  • Contact: Email: zhaoyanyan41@163.com (Yanyan Zhao)zhangjianjun@cug.edu.cn (Jianjun Zhang)
  • Supported by:
    National Natural Science Foundation of China(22409128); National Natural Science Foundation of China(22378103)

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摘要：

光催化氧还原反应(ORR)为过氧化氢(H2O2)的生产提供了一种温和且经济高效的方法。然而，催化剂的快速载流子复合和氧气吸附能力不足严重制约了其实际应用。针对上述问题，本研究提出了一种协同策略，首先通过制备富含S空位的CdIn2S4(Sv–CIS)促进电荷分离，随后负载纳米金颗粒(Au–Sv–CIS)以增强O2吸附能力。结果表明，优化后的Au–Sv–CIS在10%乙醇/水溶液中的H2O2产率显著提高至2542 μmol·h−1·g−1，分别是单体CIS和Sv–CIS的12.8倍和1.7倍。采用光致发光光谱、时间分辨光致发光光谱、瞬态光电流响应、电化学阻抗谱和飞秒瞬态吸收光谱等证明了Au–Sv–CIS具有显著改善的电荷分离效率。程序升温脱附实验和密度泛函理论计算揭示了Au–Sv–CIS增强的氧气吸附特性。本研究为实现高效的太阳能-化学能转化提供了新的设计思路。

关键词: S空位, 电荷分离, O2吸附, CdIn2S4, 过氧化氢

Abstract:

Photocatalytic oxygen reduction reaction (ORR) offers a mild and cost-effective approach for hydrogen peroxide (H2O2) production. However, its practical application is significantly hindered by rapid charge carrier recombination and insufficient O2 adsorption capacity in photocatalysts. To address these limitations, we developed a strategy involving the creation of S-vacancy-rich CdIn2S4 (Sv–CIS) to facilitate charge separation and subsequent deposition of Au nanoparticles on its surface (Au–Sv–CIS) to strengthen O2 adsorption. The results suggest that the optimized Au–Sv–CIS achieves a significantly increased H2O2 production yield of 2542 μmol·h−1·g−1 in 10%-ethanol/water solution, which is about 12.8 and 1.7 times higher than that of pure CIS and Sv–CIS. Comprehensive characterizations including photoluminescence spectra, time-resolved photoluminescence spectra, transient photocurrent response, electrochemical impedance spectra, and femtosecond transient absorption spectroscopy confirm the improved charge dynamics of Au–Sv–CIS. In addition, temperature-programmed desorption of O2 combined with density functional theory calculations conclusively demonstrates the superior O2 adsorption capacity of Au–Sv–CIS. This work provides a design strategy for efficient solar-to-chemical energy conversion through cooperative photocatalyst engineering.

Key words: S vacancy, Charge separation, O2 adsorption, CdIn2S4, Hydrogen peroxide