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Tailoring activation sites of metastable distorted 1T′-phase MoS2 by Ni doping for enhanced hydrogen evolution

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Abstract

Heteroatom doping is a promising approach to enhance catalytic activity by modulating physical properties, electronic structure, and reaction pathway. Herein, we demonstrate that appropriate Ni-doping could trigger a preferential transition of the basal plane from 2H (trigonal prismatic) to 1T′ (clustered Mo) by inducing lattice distortion and S vacancy (SV) and thus dramatically facilitate its catalytic hydrogen evolution activity. It is noteworthy that the unique catalysts did possess superior catalytic performance of hydrogen evolution reaction (HER). The rate of photocatalytic hydrogen evolution could reach 20.45 mmol·g−1·h−1 and reduced only slightly in the long period of the photocatalytic process. First-principles calculations reveal that the distorted Ni-1T′-MoS2 with SV could generate favorable water adsorption energy (Ead(H2O)) and Gibbs free energy of hydrogen adsorption (ΔGH). This work exhibits a facile and promising pathway for synergistically regulating physical properties, electronic structure, or wettability based on the doping strategy for designing HER electrocatalysts.

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Acknowledgements

This work was financially supported by the National Funds for Distinguished Young Scientists (No. 61825503), the National Natural Science Foundation of China (Nos. 51902101, 61775101, and 61804082), the Natural Science Foundation of Jiangsu Province (Nos. BK20201381 and BK20210577), the Science Foundation of Nanjing University of Posts and Telecommunications (No. NY219144), and the National College Student Innovation and Entrepreneurship Training Program.

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  1. Mingming Liu, Hengxu Li, and Shijie Liu contributed equally to this work.

Authors and Affiliations

  1. College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications, Nanjing, 210023, China

    Mingming Liu, Hengxu Li, Shijie Liu, Longlu Wang, Chun Sun, Jin Wang, Meng Tang, Shujiang Sun & Qiang Zhao

  2. State Key Laboratory of Organic Electronics and Information Displays & Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM) & Institute of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications, Nanjing, 210023, China

    Lingbin Xie, Shujuan Liu & Qiang Zhao

  3. Department of Chemistry, Tsinghua University, Beijing, 100084, China

    Zechao Zhuang

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  1. Mingming Liu
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  2. Hengxu Li
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Correspondence to Longlu Wang, Jin Wang or Qiang Zhao.

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Liu, M., Li, H., Liu, S. et al. Tailoring activation sites of metastable distorted 1T′-phase MoS2 by Ni doping for enhanced hydrogen evolution. Nano Res. 15, 5946–5952 (2022). https://doi.org/10.1007/s12274-022-4267-9

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