Targeted construction of high-performance single-atom platinum-based electrocatalysts for hydrogen evolution reaction

IF 17.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2025-02-01 Epub Date: 2025-03-04 DOI:10.1016/S1872-2067(24)60199-3
Jing Liu , Xiandi Ma , Jeonghan Roh , Dongwon Shin , Ara Cho , Jeong Woo Han , Jianping Long , Zhen Zhou , Menggai Jiao , Kug-Seung Lee , EunAe Cho
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Abstract

Exploring platinum single-atom electrocatalysts (SACs) is of great significance for effectively catalyzing the hydrogen evolution reaction in order to maximize the utilization of metal atoms. Herein, ruthenium clusters with several atoms (Rux) supported on nitrogen-doped, cost-efficient Black Pearls 2000 (RuxNBP), were synthesized as initial materials via a simple hydrothermal method. Then, [PtCl4]2– ion was reductively deposited on RuxNBP to obtain a Pt SAC (Pt1/RuxNBP). Electrochemical measurements demonstrate the excellent HER performance of Pt1/RuxNBP with a 5.7-fold increase in mass activity compared to the commercial Pt/C at 20 mV. Moreover, the cell voltage of the proton exchange membrane electrolyzer with Pt1/RuxNBP is 20 mV lower compared to that with commercial Pt/C at 1.0 A cm−2. Physical characterization and density functional theory calculations revealed that the preserved Pt–Cl bond of [PtCl4]2– and the RuxNBP support co-regulate the 5d state of isolated Pt atoms and enhance the catalytic HER capacity of Pt1/RuxNBP.
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高性能单原子铂基析氢电催化剂的定向构建
探索铂单原子电催化剂对于有效催化析氢反应,最大限度地利用金属原子具有重要意义。本文通过简单的水热法合成了氮掺杂、经济高效的黑珍珠2000 (RuxNBP)上的多原子钌团簇(Rux)作为初始材料。然后将[PtCl4]2 -离子还原沉积在RuxNBP上,得到Pt SAC (Pt1/RuxNBP)。电化学测量表明,Pt1/RuxNBP具有优异的she性能,在20 mV时,其质量活性比商用Pt/C提高了5.7倍。此外,在1.0 A cm−2时,Pt1/RuxNBP质子交换膜电解槽的电池电压比商用Pt/C低20 mV。物理表征和密度泛函理论计算表明,[PtCl4]2 -保留的Pt - cl键和RuxNBP载体共同调节了分离Pt原子的5d态,增强了Pt1/RuxNBP催化HER的能力。
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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