Key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

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外文摘要：The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron accessibility.With hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of catalysts.However,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic activity.Herein we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS2)electronic bandgap via a simple solvothermal method.We demonstrate that the conductivity of catalysts greatly affects the overall catalytic activity.We further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to reactant.Theoretical and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing energy.Our results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

外文关键词：

conductivitymolybdenum disulfidecatalytic interfaceelectron accessibilityhydrogen evolutioncharge transfer

作者：

Dongchen Han、Nanxing Gao、Yuyi Chu、Zhaoping Shi、Ying Wang、Junjie Ge、Meiling Xiao、Changpeng Liu、Wei Xing

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作者单位：

State Key Laboratory of Electroanalytical Chemistry,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China

School of Applied Chemistry and Engineering,University of Science and Technology of China,Hefei 230026,China

Laboratory of Advanced Power Sources,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China

Jilin Province Key Laboratory of Low Carbon Chemical Power Sources,Changchun 130022,China

State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China

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基金：

Strategic Priority Research Program of the Chinese Academy of SciencesInstrument Developing Project of the Chinese Academy of Sciences,and the Jilin Province Science and Technology Development PInstrument Developing Project of the Chinese Academy of Sciences,and the Jilin Province Science and Technology Development PInstrument Developing Project of the Chinese Academy of Sciences,and the Jilin Province Science and Technology Development P

项目编号：

XDA2109040020210301008GX20200201001JC20210502002ZP

出版年：

2024

DOI：

10.1007/s12274-023-6229-2

纳米研究(英文版)

CSTPCD

ISSN：

年,卷(期)：2024.17(4)

参考文献量51