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Construction of a CoRu/CoRuP Heterogeneous Electrocatalyst for Efficient pH-Universal Hydrogen Production

ACS SUSTAINABLE CHEMISTRY & ENGINEERING(2023)

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摘要
Interface modification and electronic alteration of electrocatalysts are indispensable to achieve efficient water splitting for hydrogen production. Herein, a greatly efficient, pH-universal electrocatalyst for hydrogen production is reported by resourcefully introducing the heterointerface and heteroatom with two-step electrodeposition processes. The established cobalt-doped Ru/RuP4 nanoheterostructure (CoRu/CoRuP) electrocatalyst demonstrates exceptional hydrogen evolution reaction (HER) activity and durability over a wide pH range, attaining ultralow overpotentials of 31, 30, and 24 mV at 10 mA cm(-2) in 1.0 M phosphate buffer solution (PBS), 1.0 M KOH, and 0.5 M H2SO4, respectively. The optimized electronic structure of CoRu/CoRuP is proved by detailed structural characterization and density-functional theory (DFT) calculation, implying that the d-band center shifts downward by 0.21 eV compared with that of the CoRu catalyst, which contributes to the production of hydrogen intermediates and H-desorption for the HER. In addition, interfacial modification for the CoRu/CoRuP catalyst contributes to the expansion of the electrochemical active surface and the production of hydrogen intermediates in the HER Volmer step. This research highlights the importance of interfacial properties and electronic structure in determining catalytic activity and suggests novel approaches for designing efficient, nanoscale, complex interfacial structure electrocatalysts.
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关键词
interface modification,electronic alteration,two-step deposition,pH-universal,hydrogen evolutionreaction
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