Citation: Shuang Cao, Bo Zhong, Chuanbiao Bie, Bei Cheng, Feiyan Xu. WO₃/Zn_0.5Cd_0.5S S型异质结光催化产氢耦合有机物转化机理研究[J]. Acta Physico-Chimica Sinica, ;2024, 40(5): 230701. doi: 10.3866/PKU.WHXB202307016 shu

WO₃/Zn_0.5Cd_0.5S S型异质结光催化产氢耦合有机物转化机理研究

1.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China;
2.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, China

Received Date: 11 July 2023
Revised Date: 25 July 2023
Accepted Date: 25 July 2023

Fund Project: This work was supported by the National Key Research and Development Program of China (2022YFB3803600, 2022YFE0115900), National Natural Science Foundation of China (52003213, 22238009, 22261142666, 52073223, 22278324, 51932007), and the Natural Science Foundation of Hubei Province of China (2022CFA001).

开发新型纳米材料实现光催化产氢耦合有机物转化、提高太阳能到化学能的转换效率，在解决能源和环境危机方面具有巨大潜力。三元金属硫化物具有可调控的带隙和优异的可见光响应，在光催化分解水产氢方面引起了广泛关注。其中，Zn_0.5Cd_0.5S是一种带隙较窄、导带位置较高、耐光腐蚀的还原型光催化剂；然而，单一Zn_0.5Cd_0.5S中光生电子和空穴的复合率较高，只有少部分光生载流子参与光催化反应，导致量子效率较低而无法达到实际需求。WO₃是一种典型的氧化型光催化剂，具有较低的价带位置和较强的氧化能力，是与Zn_0.5Cd_0.5S耦合构建S型异质结的理想半导体。基于此，本文通过静电纺丝和水热方法将Zn_0.5Cd_0.5S纳米片垂直生长在WO₃纳米纤维上，制备了具有核壳结构的WO₃/Zn_0.5Cd_0.5S异质结。功函数的差异驱动Zn_0.5Cd_0.5S的电子转移到WO₃上，在界面处形成内建电场并使能带弯曲。通过原位光照X射线光电子能谱、电子顺磁共振和时间分辨荧光光谱分析，发现在内建电场、弯曲能带和库仑吸引力的作用下，WO₃导带上的光生电子迁移到Zn_0.5Cd_0.5S价带上并与其光生空穴复合，表明WO₃和Zn_0.5Cd_0.5S之间形成了S型异质结，实现了具有强氧化还原能力的载流子的高效分离。得益于独特的S型光催化机制以及反应物在催化剂表面的有效吸附与活化，没有贵金属助催化剂的情况下，WO₃/Zn_0.5Cd_0.5S异质结在产氢(715 μmol·g^-1·h^-1)和乳酸转化为丙酮酸方面表现出增强的光催化活性，实现了光生电子和空穴的高效利用。原位漫反射傅里叶变换红外光谱和密度泛函理论计算揭示了光催化产氢和有机物转化的反应机理。本工作为设计和研究新型S型异质结光催化剂、实现高效产氢耦合有机物转化提供了新的见解。
- Tungsten oxide,
- S-scheme heterojunction,
- Hydrogen production,
- Organic transformation,
- Chemisorption and activation
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WO3/Zn0.5Cd0.5S S型异质结光催化产氢耦合有机物转化机理研究

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WO₃/Zn_0.5Cd_0.5S S型异质结光催化产氢耦合有机物转化机理研究