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

引用本文: 赵艳艳, 吴珍, 张勇, 朱必成, 张建军. 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[J]. 物理化学学报, 2025, 41(11): 100142. doi: 10.1016/j.actphy.2025.100142 shu

Citation: Yanyan Zhao, Zhen Wu, Yong Zhang, Bicheng Zhu, Jianjun Zhang. Enhancing photocatalytic H₂O₂ production via dual optimization of charge separation and O₂ adsorption in Au-decorated S-vacancy-rich CdIn₂S₄[J]. Acta Physico-Chimica Sinica, 2025, 41(11): 100142. doi: 10.1016/j.actphy.2025.100142 shu

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.
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

通讯作者: 赵艳艳, zhaoyanyan41@163.com; 张建军, zhangjianjun@cug.edu.cn

基金项目:
国家自然科学基金 22409128

国家自然科学基金 22378103

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(S_v–CIS)促进电荷分离，随后负载纳米金颗粒(Au–S_v–CIS)以增强O₂吸附能力。结果表明，优化后的Au–S_v–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S_v–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–S_v–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–S_v–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:

English

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

Yanyan Zhao ^{1,
,} ,
Zhen Wu ^1, ,
Yong Zhang ^2, ,
Bicheng Zhu ^3, ,
Jianjun Zhang ^{3,
,}

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

Corresponding author: Email: zhaoyanyan41@163.com (Y. Zhao); Email: zhangjianjun@cug.edu.cn (J.J. Zhang)

Received Date: 30 June 2025
Accepted Date: 29 July 2025
Revised Date: 28 July 2025
Available Online: 15 November 2025
Fund Project:
National Natural Science Foundation of China

National Natural Science Foundation of China

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 (S_v–CIS) to facilitate charge separation and subsequent deposition of Au nanoparticles on its surface (Au–S_v–CIS) to strengthen O₂ adsorption. The results suggest that the optimized Au–S_v–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 S_v–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–S_v–CIS. In addition, temperature-programmed desorption of O₂ combined with density functional theory calculations conclusively demonstrates the superior O₂ adsorption capacity of Au–S_v–CIS. This work provides a design strategy for efficient solar-to-chemical energy conversion through cooperative photocatalyst engineering.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: 赵艳艳, zhaoyanyan41@163.com; 张建军, zhangjianjun@cug.edu.cn

English

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

Corresponding author: Email: zhaoyanyan41@163.com (Y. Zhao); Email: zhangjianjun@cug.edu.cn (J.J. Zhang)

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