Low-valence platinum single atoms in sulfur-containing covalent organic frameworks for photocatalytic hydrogen evolution

Liangjun Chen, Guinan Chen, Chengtao Gong, Yifei Zhang, Zhihao Xing, Jiahao Li, Guodong Xu, Gao Li () and Yongwu Peng ()
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Liangjun Chen: Zhejiang University of Technology
Guinan Chen: Zhejiang University of Technology
Chengtao Gong: Zhejiang University of Technology
Yifei Zhang: Shenyang Normal University
Zhihao Xing: Zhejiang University of Technology
Jiahao Li: Zhejiang University of Technology
Guodong Xu: Yancheng Teachers University
Gao Li: Shenyang Normal University
Yongwu Peng: Zhejiang University of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract This study focuses on optimizing catalytic activity in photocatalytic hydrogen evolution reaction by precisely designing and modulating the electronic structure of metal single atoms. The catalyst, denoted as PtSA@S-TFPT, integrates low-valence platinum single atoms into sulfur-containing covalent organic frameworks. The robust asymmetric four-coordination between sulfur and platinum within the framework enables a high platinum loading of 12.1 wt%, resulting in efficient photocatalytic hydrogen production activity of 11.4 mmol g−1 h−1 and stable performance under visible light. These outcomes are attributed to a reduced hydrogen desorption barrier and enhanced photogenerated charge separation, as indicated by density functional theory calculations and dynamic carrier analysis. This work challenges traditional notions and opens an avenue for developing low-valence metal single atom-loaded covalent organic framework catalysts to advance photocatalytic hydrogen evolution.

Date: 2024
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DOI: 10.1038/s41467-024-54959-8

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