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; Yongwu Peng

doi:10.1038/s41467-024-54959-8

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

Nat Commun. 2024 Dec 3;15(1):10501. doi: 10.1038/s41467-024-54959-8.

Authors

Liangjun Chen^#¹, Guinan Chen^#¹, Chengtao Gong^#¹, Yifei Zhang², Zhihao Xing¹, Jiahao Li¹, Guodong Xu³, Gao Li^{4

5}, Yongwu Peng⁶

Affiliations

¹ College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, China.
² Institute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang, Liaoning, China.
³ College of Chemical and Environmental Engineering, Yancheng Teachers University, Yancheng, Jiangsu, China.
⁴ Institute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang, Liaoning, China. gaoli@dicp.ac.cn.
⁵ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, China. gaoli@dicp.ac.cn.
⁶ College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, China. ywpeng@zjut.edu.cn.

^# Contributed equally.

PMID: 39627232
DOI: 10.1038/s41467-024-54959-8

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.

Abstract

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