Enhanced hydrogen evolution of single-atom Ru sites via geometric and electronic engineering: N and S dual coordination

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作者
Wang, Min Jie [1 ]
Ji, Muwei [1 ]
Zheng, Xingqun [2 ]
Jiang, Chi [1 ]
Zhao, Hang [1 ]
Mao, Zhan Xin [3 ]
Zhang, Minghui [1 ]
Zhu, Caizhen [1 ]
Xu, Jian [1 ]
机构
[1] Institute of Low-dimensional Materials Genome Initiative, College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen,Guangdong,518060, China
[2] School of Chemistry and Chemical Engineering, Chongqing University, Shazhengjie 174, Chongqing,400044, China
[3] China Automotive Engineering Research Institute Co Ltd, No. 9 Jinyu Avenue, Chongqing,401122, China
基金
中国国家自然科学基金;
关键词
Catalyst activity - Cyclic voltammetry - Hydrogen - Atoms - Coordination reactions - Hydrogen bonds;
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摘要
Single-atom catalysts (SACs) have attracted wide attention, however a challenge in both the synthesis and determination of such active sites still occurs. Here a simply one-pot hydrothermal method has been reported to prepare SACs based on strong dual-coordinated interactions. The comprehensive structure analysis uncloses the highly dispersed single-atom Ru (RuSA) sites and formation of Ru–N and Ru–S bonds, suggesting the strong Ru-support interactions. The achieved catalyst Ru/N,S-Go shows robust hydrogen evolution reaction (HER) performances with a low overpotential 26 mV at a typical 10 mA cm−2 of current density, 30 mV of Tafel slope and excellent durability of continuous 10,000 cyclic voltammetry cycles, outperforming the benchmark commercial Pt/C. The density functional theory (DFT) calculations uncover that the strong coordination of Ru–N and Ru–S bonds could be not only efficient to water splitting, but then promote the formation of adsorbed hydrogen to hydrogen molecules (H* → H2), implying ultrahigh inherent HER activity. We believe that this work could provide a new idea for preparation of other SACs applied in different electrochemical fields. © 2021 Elsevier B.V.
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