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Multi-interface collaboration of graphene cross-linked NiS-NiS2-Ni3S4 polymorph foam towards robust hydrogen evolution in alkaline electrolyte

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Abstract

Electrocatalytic hydrogen production in alkaline media is extensively adopted in industry. Unfortunately, further performance improvement is severely impeded by the retarded kinetics, which requires the fine regulation of water dissociation, hydrogen recombination, and hydroxyl desorption. Herein, we develop a multi-interface engineering strategy to make an elaborate balance for the alkaline hydrogen evolution reaction (HER) kinetics. The graphene cross-linked three-phase nickel sulfide (NiS-NiS2-Ni3S4) polymorph foam (G-NNNF) was constructed through hydrothermal sulfidation of graphene wrapped nickel foam as a three-dimensional (3D) scaffold template. The G-NNNF exhibits superior catalytic activity toward HER in alkaline electrolyte, which only requires an overpotential of 68 mV to drive 10 mA·cm−2 and is better than most of the recently reported metal sulfides catalysts. Density functional theory (DFT) calculations verify the interfaces between nickel sulfides (NiS/NiS2/Ni3S4) and cross-linked graphene can endow the electrocatalyst with preferable hydrogen adsorption as well as metallic nature. In addition, the electron transfer from Ni3S4/NiS2 to NiS results in the electron accumulation on NiS and the hole accumulation on Ni3S4/NiS2, respectively. The electron accumulation on NiS favors the optimization of the H* adsorption, whereas the hole accumulation on Ni3S4 is beneficial for the adsorption of H2O. The work about multi-interface collaboration pushes forward the frontier of excellent polymorph catalysts design.

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Acknowledgements

This work was supported by the National Key Research and Development Program of China (No. 2017YFB0405400), Shandong Provincial Natural Science Foundation (Nos. ZR2019BB025 and ZR2018ZC0842), the Project of “20 items of University” of Jinan (No. 2018GXRC031), the National Natural Science Foundation of China (Nos. 21976014, U1930402 and 22071172), and the generous computer time from TianHe2-JK Supercomputer Center.

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  1. Haiqing Wang and Wenjing Zhang contributed equally to this work.

Authors and Affiliations

  1. Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, Institute for Advanced Interdisciplinary Research (iAIR), University of Jinan, Jinan, 250022, China

    Haiqing Wang, Xiaowei Zhang, Weijia Zhou & Hong Liu

  2. Beijing Computational Science Research Center, Beijing, 100193, China

    Wenjing Zhang & Shuxian Hu

  3. Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China

    Zhicheng Zhang

  4. State Key Laboratory of Crystal Materials, Shandong University, Jinan, 250100, China

    Hong Liu

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  1. Haiqing Wang
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  2. Wenjing Zhang
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  3. Xiaowei Zhang
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  4. Shuxian Hu
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  5. Zhicheng Zhang
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Correspondence to Haiqing Wang, Shuxian Hu or Hong Liu.

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12274_2021_3445_MOESM1_ESM.pdf

Multi-interface collaboration of graphene cross-linked NiS-NiS2-Ni3S4 polymorph foam towards robust hydrogen evolution in alkaline electrolyte

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Wang, H., Zhang, W., Zhang, X. et al. Multi-interface collaboration of graphene cross-linked NiS-NiS2-Ni3S4 polymorph foam towards robust hydrogen evolution in alkaline electrolyte. Nano Res. 14, 4857–4864 (2021). https://doi.org/10.1007/s12274-021-3445-5

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