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Research Article

Accelerating water dissociation at carbon supported nanoscale Ni/NiO heterojunction electrocatalysts for high-efficiency alkaline hydrogen evolution

Cong Li1,2, Jiang-Yan Xue1, Wei Zhang1, Fei-Long Li3( ), Hongwei Gu1, Pierre Braunstein4, Jian-Ping Lang1,2( )
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China
State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai 200032, China
School of Chemistry and Materials Engineering, Changshu Institute of Technology, Changshu 215500, China
Université de Strasbourg-CNRS, Institut de Chimie (UMR 7177 CNRS), 4 rue Blaise Pascal-CS 90032, Strasbourg 67081, France
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Graphical Abstract

The Ni/NiO heterojunction porous graphitic carbon (Ni/NiO-PGC10-1-400) obtained by hydrogen reduction pyrolysis of Ni-metal-organic framework (MOF) exhibits excellent alkaline hydrogen evolution reaction (HER) activity and long-term stability (η10 = 30 mV, 65 h), due to promoting water dissociation (Volmer step) and optimizing Ni adsorption energy for H* (Heyrovsky/Tafel step) by NiO, more accessible active sites and accelerating electron transport by PGC.

Abstract

The synergistic catalysis of heterojunction electrocatalysts for the multi-step process in hydrogen evolution reaction (HER) is a promising approach to enhance the kinetics of alkaline HER. Herein, we proposed a strategy to form nanoscale Ni/NiO heterojunction porous graphitic carbon composites (Ni/NiO-PGC) by reduction-pyrolysis of the preformed Ni-metal-organic framework (MOF) under H2/N2 atmosphere. Benefiting from low electron transfer resistance, increased number of active sites, and unique hierarchical micro-mesoporous structure, the optimized Ni/NiO-PGC10-1-400 exhibited excellent electrocatalytic performance and robust stability for alkaline HER (η10 = 30 mV, 65 h). Density functional theory (DFT) studies revealed that the redistribution of electrons at the Ni/NiO interface enables the NiO phase to easily initiate the dissociation of alkaline H2O, and shifts down the d-band center of Ni and optimizes the H* adsorption–desorption process of Ni, thereby leading to extremely high HER activity. This work contributes to a further understanding of the synergistic promotion of the multi-step HER processes by heterojunction electrocatalysts.

Keywords

water dissociationNi/NiO heterojunctionmetal-organic frameworks (MOFs) derivativeshydrogen evolution reactionreduction pyrolysis

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Nano Research
Volume 16 Issue 4,
April 2023
Pages 4742-4750
DOI: 10.1007/s12274-022-5194-5
Cite this article:
Li C, Xue J-Y, Zhang W, et al. Accelerating water dissociation at carbon supported nanoscale Ni/NiO heterojunction electrocatalysts for high-efficiency alkaline hydrogen evolution. Nano Research, 2023, 16(4): 4742-4750. https://doi.org/10.1007/s12274-022-5194-5
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Received: 18 August 2022
Revised: 26 September 2022
Accepted: 11 October 2022
Published: 15 December 2022
© Tsinghua University Press 2022
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