Citation: Shuang Cao, Bo Zhong, Chuanbiao Bie, Bei Cheng, Feiyan Xu. Insights into Photocatalytic Mechanism of H₂ Production Integrated with Organic Transformation over WO₃/Zn_0.5Cd_0.5S S-Scheme Heterojunction[J]. Acta Physico-Chimica Sinica, ;2024, 40(5): 230701. doi: 10.3866/PKU.WHXB202307016 shu

Insights into Photocatalytic Mechanism of H₂ Production Integrated with Organic Transformation over WO₃/Zn_0.5Cd_0.5S S-Scheme Heterojunction

Shuang Cao ¹ ,
Bo Zhong ¹ ,
Chuanbiao Bie ² ,
Bei Cheng ¹ ,
Feiyan Xu ^2,,

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

Corresponding author: Feiyan Xu, xufeiyan@cug.edu.cn
Received Date: 11 July 2023
Revised Date: 25 July 2023
Accepted Date: 25 July 2023
Available Online: 31 July 2023
Fund Project: the National Key Research and Development Program of China 2022YFB3803600the National Key Research and Development Program of China 2022YFE0115900National Natural Science Foundation of China 52003213National Natural Science Foundation of China 22238009National Natural Science Foundation of China 22261142666National Natural Science Foundation of China 52073223National Natural Science Foundation of China 22278324National Natural Science Foundation of China 51932007the Natural Science Foundation of Hubei Province of China 2022CFA001

Developing novel nanostructures to enhance the efficiency of solar-to-chemical conversion through integrated photocatalytic hydrogen (H₂) evolution and organic transformation holds great promise in addressing pressing energy and environmental crises. Ternary metal sulfides have garnered considerable attention in photocatalytic H₂ production due to their tunable bandgap and excellent visible light response. Among them, Zn_0.5Cd_0.5S stands out as a reduction photocatalyst with a narrow bandgap, a high conduction band level, and excellent resistance to photocorrosion. However, unitary Zn_0.5Cd_0.5S suffers from a high recombination rate of photogenerated electron/hole pairs, resulting in only a small fraction of charge carriers being involved in the photoreactions, leading to a low quantum efficiency that falls short of practical demand. WO₃, a typical oxidation photocatalyst with a lower valence band position and strong oxidization ability, is an ideal candidate for constructing an S-scheme heterojunction with Zn_0.5Cd_0.5S. Herein, a core-shell structured WO₃/Zn_0.5Cd_0.5S heterojunction with Zn_0.5Cd_0.5S nanosheets vertically growing out of WO₃ nanofibers is fabricated through electrospinning and hydrothermal methods. The distinct disparity in work functions leads to the transfer of electrons from Zn_0.5Cd_0.5S to WO₃ upon contact, creating an interfacial electric field (IEF) and simultaneously bending the energy bands at the interface. As a consequence of IEF, bent energy bands, and coulomb attraction, the photogenerated electrons in the conduction band of WO₃ migrate to the valence band of Zn_0.5Cd_0.5S and recombine with its photoinduced holes, signifying the formation of an S-scheme heterojunction between WO₃ and Zn_0.5Cd_0.5S and enabling efficient separation of powerful charge carriers, as evidenced by in situ irradiated X-ray photoelectron spectroscopy, electron paramagnetic resonance, and time-resolved fluorescence spectroscopy analyses. Benefiting from the unique S-scheme photocatalytic mechanism, along with the effective chemisorption and activation of reactants on the catalyst, the optimized WO₃/Zn_0.5Cd_0.5S heterostructures exhibit exceptional photocatalytic performance in H₂ production (715 μmol∙g⁻¹∙h⁻¹) and the transformation from lactic acid to pyruvic acid without the need for any noble metal cocatalyst, achieving the full utilization of photoinduced electrons and holes. In situ diffuse reflectance infrared Fourier transform spectroscopy, as well as density functional theory simulations, reveal the photoreaction mechanism of H₂ production and organic transformation. This work offers valuable insights into the design and investigation of the mechanism behind novel S-scheme heterojunction photocatalysts, enabling high-performance H₂ production and simultaneous organic transformation.
- Tungsten oxide,
- S-scheme heterojunction,
- Hydrogen production,
- Organic transformation,
- Chemisorption and activation
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Insights into Photocatalytic Mechanism of H2 Production Integrated with Organic Transformation over WO3/Zn0.5Cd0.5S S-Scheme Heterojunction

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通讯作者: 陈斌, bchen63@163.com

Insights into Photocatalytic Mechanism of H₂ Production Integrated with Organic Transformation over WO₃/Zn_0.5Cd_0.5S S-Scheme Heterojunction