Citation: Xinyu Miao, Hao Yang, Jie He, Jing Wang, Zhiliang Jin. Adjusting the electronic structure of Keggin-type polyoxometalates to construct S-scheme heterojunction for photocatalytic hydrogen evolution[J]. Acta Physico-Chimica Sinica, ;2025, 41(6): 100051. doi: 10.1016/j.actphy.2025.100051 shu

Adjusting the electronic structure of Keggin-type polyoxometalates to construct S-scheme heterojunction for photocatalytic hydrogen evolution

Xinyu Miao ¹ ,
Hao Yang ^1,3 ,
Jie He ¹ ,
Jing Wang ² ,
Zhiliang Jin ¹

1.
School of Chemistry and Chemical Engineering, Ningxia Key Laboratory of Solar Chemical Conversion Technology, Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University, Yinchuan 750021, China;
2.
School of Materials Science & Engineering, Tianjin University of Technology, Tianjin 300384, China;
3.
College of Chemical Engineering, Fuzhou University, Fuzhou 350116, China

Received Date: 25 November 2024
Revised Date: 10 January 2025
Accepted Date: 13 January 2025

Fund Project: The project was supported by the Innovative Team for Transforming Waste Cooking Oil into Clean Energy and High Value-Added Chemicals of China and Ningxia Low-Grade Resource High Value Utilization And Environmental Chemical Integration Technology Innovation Team Project of Ningxia.

The sluggish electron migration rate and pronounced electron-hole recombination, pose significant obstacles to achieving high photocatalytic efficiency. The utilization of multiple catalysts for the construction of heterojunctions can effectively enhance charge separation. A series of Keggin-type hollow dodecahedral polyoxometalates were prepared via hydrothermal synthesis, and their molecular orbitals were modified through the addition of metal elements. The incorporation of metal elements modulated the electronic structure of polyoxometalates, effectively enhancing the electron aggregation capability of polyoxometalates. Single-component catalysts often face serious hole-electron recombination. In order to solve this problem, the scheme of constructing heterojunction is proposed to improve the electron transport efficiency. By immobilizing ZnCdS nanoparticles onto the polyoxometalate surface, the heterojunction architecture was engineered to significantly enhance the interfacial charge transfer capability. Density Functional Theory (DFT) calculations and the experimental results indicate that the modulation of metallic components renders the polyoxometalate a more favorable energy-level orbital. The catalytic mechanism of ZnCdS and KMoP S-scheme heterojunction was also verified. The formation of S-scheme heterojunctions further improves the electron transfer efficiency compared to other traditional heterojunctions, achieving efficient utilization of photo generated electrons and holes. Additionally, the S-scheme heterojunction shifts the catalyst's d-band center closer to the Fermi level, thereby improving electrical conductivity. This article provides a new approach for energy level regulation of polyoxometalates and the design of S-scheme heterojunctions.
- ZnCdS,
- Keggin-type polyoxometalates,
- Hollow structure,
- Charge density difference,
- d band center adjustment,
- S-scheme heterojunction
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