Citation: Yi Yang, Xin Zhou, Miaoli Gu, Bei Cheng, Zhen Wu, Jianjun Zhang. Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn₂S₄ photocatalyst for H₂O₂ production and benzylamine oxidation[J]. Acta Physico-Chimica Sinica, ;2025, 41(6): 100064. doi: 10.1016/j.actphy.2025.100064 shu

Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn₂S₄ photocatalyst for H₂O₂ production and benzylamine oxidation

Yi Yang ^1,2 ,
Xin Zhou ³ ,
Miaoli Gu ² ,
Bei Cheng ² ,
Zhen Wu ³ ,
Jianjun Zhang ⁴

1.
School of Materials and Chemical Engineering, Hubei University of Technology, Wuhan 430068, Hubei Province, China;
2.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, Hubei Province, China;
3.
Department of Chemical Engineering, Ordos Institute of Technology, Ordos 017000, Inner Mongolia Autonomous Region, China;
4.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China

Received Date: 22 January 2025
Revised Date: 12 February 2025
Accepted Date: 13 February 2025

Fund Project: The project was supported by National Natural Science Foundation of China (22278324, 52202375, 22469001) and the Science Foundation of Hubei Province of China (2022CFA001).

Photocatalytic hydrogen peroxide (H₂O₂) production is a crucial process for clean energy conversion, involving the reduction of O₂ through two electrons. However, this process is often hampered by the sluggish water oxidation involving the photogenerated holes. To address this challenge, we have constructed a dual-functional S-scheme ZnO/CdIn₂S₄ heterojunction systerm coupling the H₂O₂ generation with a value-added benzylamine (BA) oxidation reaction. In this dual-functional photocatalytic system, photogenerated electrons in CdIn₂S₄ efficiently reduce O₂ to produce H₂O₂, while photogenerated holes in ZnO selectively oxidize BA to N-benzylidenebenzylamine. Leveraging the advantages of the S-scheme heterojunction, the optimized ZnO/CdIn₂S₄ photocatalyst displays an enhanced H₂O₂ production rate (386 μmol·L^-1·h^-1) and BA oxidation fraction (81%) than pure ZnO or CdIn₂S₄. Femtosecond transient absorption (fs-TA) spectroscopy confirm the ultrafast S-scheme electron transfer from the ZnO conduction band (CB) to the CdIn₂S₄ valence band (VB) upon photoexcitation of the ZnO/CdIn₂S₄ composite. Besides, timely depletion of VB holes in ZnO and CB electrons in CdIn₂S₄ can accelerate the interfacial electron transfer in the ZnO/CdIn₂S₄ S-scheme heterojunction. The innovative design of the ZnO/CdIn₂S₄ S-scheme photocatalyst provides new insights for developing efficient dual-functional heterojunction photocatalytic systems and introduces a novel method for studying S-scheme heterojunctions using fs-TA spectroscopy.
- Photocatalytic H₂O₂ production,
- S-scheme heterojunction,
- Selective benzylamine oxidation,
- fs-TA spectroscopy,
- Electron transfer dynamics
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沈阳化工大学材料科学与工程学院沈阳 110142

Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn2S4 photocatalyst for H2O2 production and benzylamine oxidation

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通讯作者: 陈斌, bchen63@163.com

Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn₂S₄ photocatalyst for H₂O₂ production and benzylamine oxidation