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

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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.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22271203, 21773163, and 22001021), the State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry (No. KF2021005), the Natural Science Foundation of Jiangsu Province (No. BK20201048), the Natural Science Research Project of Higher Education Institutions in Jiangsu Province (No. 20KJB150008), the Collaborative Innovation Center of Suzhou Nano Science and Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions, and the Project of Scientific and Technologic Infrastructure of Suzhou (No. SZS201905). We are grateful to the useful comments and suggestions from the editor and the reviewers.

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  1. College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, 215123, China

    Cong Li, Jiang-Yan Xue, Wei Zhang, Hongwei Gu & Jian-Ping Lang

  2. State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai, 200032, China

    Cong Li & Jian-Ping Lang

  3. School of Chemistry and Materials Engineering, Changshu Institute of Technology, Changshu, 215500, China

    Fei-Long Li

  4. Institut de Chimie (UMR 7177 CNRS), Université de Strasbourg-CNRS, 4 rue Blaise Pascal-CS 90032, Strasbourg, 67081, France

    Pierre Braunstein

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

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Li, C., Xue, JY., Zhang, W. et al. Accelerating water dissociation at carbon supported nanoscale Ni/NiO heterojunction electrocatalysts for high-efficiency alkaline hydrogen evolution. Nano Res. 16, 4742–4750 (2023). https://doi.org/10.1007/s12274-022-5194-5

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