Immortally Dual Sites on Single-Atom Dispersed Electrocatalyst for High-Efficient Hydrogen/Oxygen Evolution Reaction

Huachuan Sun, Chine-Wei Tung, Yang Qiu, Wei Zhang, Qi Wang, Zhishan Li, Jiang Tang, Hsiao‐Chien Chen, Chundong Wang, Hao Ming Chen
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Abstract

Real bifunctional electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) should be the ones that exhibit an immortal behavior during catalysis without structural transformation or surface reconstruction. Otherwise, they could be only termed as “pre-catalysts” rather than the real catalysts. Herein, single-atom dispersed catalysts (SACs) embedding atomically dispersed Ru onto nickel-vanadium layered double hydroxide matrix (termed as Ru/Ni3V-LDH) not only exhibit excellent HER activity (~ 54.3 fold mass activity vs. the commercial Pt/C) and OER activity, but also possess decent full-cell performance for overall water splitting (1.5 V@10 mA cm-2). Most importantly, in-situ XAS and Raman spectroscopic studies clarified that, unlike numerous bifunctional catalysts that have suffered from the structural reconstruction/transformation for adapting the HER/OER cycles, Ru/Ni3V-LDH is characteristic of immortally dual reactive sites  (i.e., Ru and Ni sites) for individual catalysis of electrochemical water splitting and could be termed as the real bifunctional electrocatalyst.
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高效析氢/析氧反应的单原子分散电催化剂的不朽双位点
真正用于析氢反应和析氧反应的双官能团电催化剂应该是在催化过程中不发生结构转变或表面重构而表现出不朽行为的电催化剂。否则,它们只能被称为“预催化剂”,而不是真正的催化剂。本研究中,单原子分散催化剂(SACs)将原子分散的Ru嵌入镍钒层状双氢氧化物基体(称为Ru/Ni3V-LDH)上,不仅表现出优异的HER活性(质量活性是商业Pt/C的54.3倍)和OER活性,而且还具有良好的全电池整体水分解性能(1.5 V@10 mA cm-2)。最重要的是,原位XAS和拉曼光谱研究表明,与许多双功能催化剂不同,为了适应HER/OER循环而遭受结构重构/转变,Ru/Ni3V-LDH具有永久的双活性位点(即Ru和Ni位点),用于单独催化电化学水分解,可以被称为真正的双功能电催化剂。
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