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Research Article

Collaborative effect between single-atom Re and S vacancy on modulating localized electronic structure of MoS2 catalysts for alkaline hydrogen evolution

Yajing Zhang1,2,3,4, Xingkun Wang1,2,3, Xiangju Song1,2,3, Heqing Jiang1,2,3( )
Key Laboratory of Functional Membrane Material and Membrane Technology, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China
Shandong Energy Institute, Qingdao 266101, China
Qingdao New Energy Shandong Laboratory, Qingdao 266101, China
University of Chinese Academy of Sciences, Beijing 100049, China
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Graphical Abstract

The single-atom Re and the adjacent S vacancy in MoS2 (denoted as Re-MoS2-Vs) exhibit collaborative effect on regulating the localized electronic structure of active sites (viz. Re-(S, Vs)-Mo), which endows Re-MoS2-Vs with low H2O dissociation barrier, optimized H adsorption, and the strengthened Mo–S bonds for effective and stable alkaline hydrogen evolution.

Abstract

Optimizing the catalytic activity and stability of molybdenum disulfide (MoS2) towards alkaline hydrogen evolution reaction (HER) is significant for sustaining green hydrogen. A moderate localized electronic structure of active sites plays a crucial role in determining the activity and stability of the catalysts, yet how to construct such localized electronic structure still remains indeterminacy. Enlightened by theoretical prediction, herein, the introduction of both single-atom Re and the adjacent S vacancy in MoS2 (denoted as Re-MoS2-Vs) exhibits collaborative effect on regulating the localized electronic structure of active sites (viz. Re-(S, Vs)-Mo). Such regulated electronic structure helps to decrease the energy barrier of the water dissociation and optimize hydrogen adsorption energy for enhancing alkaline HER performance. Most importantly, Mo–S bonds in the above local Re-(S, Vs)-Mo configurations are also strengthened for preventing the leaching of Mo and S atoms and then ensuring the long-time stability. Consequently, the deliberately designed Re-MoS2-Vs with a Re coordination number of ~ 5.0 is experimentally verified to exhibit a comparable electrocatalytic performance and robust operational stability over 120 h. This strategy provides a promising guidance for modulating the electronic structure of MoS2 based catalysts via double-tuning atomic-scale local configuration for HER applications.

Keywords

molybdenum disulfidelocalized electronic structureatomic Re dopingS vacancyalkaline hydrogen evolution

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Nano Research
Volume 17 Issue 11,
November 2024
Pages 9507-9517
DOI: 10.1007/s12274-024-6909-x
Cite this article:
Zhang Y, Wang X, Song X, et al. Collaborative effect between single-atom Re and S vacancy on modulating localized electronic structure of MoS2 catalysts for alkaline hydrogen evolution. Nano Research, 2024, 17(11): 9507-9517. https://doi.org/10.1007/s12274-024-6909-x
Topics:
Hydrogen evolution reaction

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Received: 22 May 2024
Revised: 08 July 2024
Accepted: 21 July 2024
Published: 30 August 2024
© Tsinghua University Press 2024
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