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Nano Research 2022, 15(7): 5946-5952 https://doi.org/10.1007/s12274-022-4267-9
Research Article | Issue | Published: 02 May 2022

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

Show Author's Information Mingming Liu1,§,  Hengxu Li1,§,  Shijie Liu1,§,  Longlu Wang1( ),  Lingbin Xie2,  Zechao Zhuang3,  Chun Sun1,  Jin Wang1( ),  Meng Tang1,  Shujiang Sun1,  Shujuan Liu2,  Qiang Zhao1,2( )
College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications, Nanjing 210023, China
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
Department of Chemistry, Tsinghua University, Beijing 100084, China

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

Keywords:
electronic structure, phase transformation, hydrogen evolution, S vacancy, Ni doping
Topics:
Catalytic
Cite this article:
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 Research, 2022, 15(7): 5946-5952. https://doi.org/10.1007/s12274-022-4267-9
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Abstract Full text Electronic supplementary material About this article

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 (∆GH). 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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Electronic supplementary material
About this article

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

Show Author's information Mingming Liu1,§, Hengxu Li1,§, Shijie Liu1,§, Longlu Wang1( ), Lingbin Xie2, Zechao Zhuang3, Chun Sun1, Jin Wang1( ), Meng Tang1, Shujiang Sun1, Shujuan Liu2, Qiang Zhao1,2( )
College of Electronic and Optical Engineering & College of Flexible Electronics (Future Technology), Nanjing University of Posts & Telecommunications, Nanjing 210023, China
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
Department of Chemistry, Tsinghua University, Beijing 100084, China

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

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 (∆GH). 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.

Keywords: electronic structure, phase transformation, hydrogen evolution, S vacancy, Ni doping

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Publication history
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Acknowledgements

Publication history

Received: 10 February 2022
Revised: 18 February 2022
Accepted: 21 February 2022
Published: 02 May 2022
Issue date: July 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

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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