含硫共价有机框架中低价铂单原子的光催化析氢

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Liangjun Chen, Guinan Chen, Chengtao Gong, Yifei Zhang, Zhihao Xing, Jiahao Li, Guodong Xu, Gao Li, Yongwu Peng
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引用次数: 0

摘要

本研究主要通过对金属单原子电子结构的精确设计和调控来优化光催化析氢反应的催化活性。催化剂(表示为PtSA@S-TFPT)将低价铂单原子整合到含硫共价有机框架中。框架内硫和铂之间强大的不对称四配位使得铂负载高达12.1%,从而产生11.4 mmol g−1 h−1的高效光催化产氢活性和可见光下稳定的性能。正如密度泛函理论计算和动态载流子分析所表明的那样,这些结果归因于氢解吸屏障的降低和光生电荷分离的增强。这项工作挑战了传统观念,为开发低价金属单原子负载共价有机框架催化剂以推进光催化析氢开辟了道路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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

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

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.

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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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