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Research Article

Strategic design and fabrication of MXenes-Ti3CNCl2@CoS2 core–shell nanostructure for high-efficiency hydrogen evolution

Jizhou Jiang1,3 ( ), Saishuai Bai1, Meiqing Yang2( ), Jing Zou1, Neng Li4, Jiahe Peng4, Haitao Wang1, Kun Xiang1, Song Liu5, Tianyou Zhai6( )
School of Environmental Ecology and Biological Engineering, School of Chemistry and Environmental Engineering, Key Laboratory of Green Chemical Engineering Process of Ministry of Education, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Wuhan Institute of Technology, Wuhan 430205, China
College of Life and Environmental Science, Hunan University of Arts and Science, Changde 415000, China
Key Laboratory of Rare Mineral, Ministry of Natural Resources, Geological Experimental Testing Center of Hubei Province, Wuhan 430034, China
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China
Institute of Chemical Biology and Nanomedicine (ICBN), State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China
State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
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Graphical Abstract

Theoretical predictions of first-principles calculations reveal that the Ti3CNCl2@CoS2 core–shell nanostructure has Gibbs free energy of hydrogen adsorption (|ΔGH|) close to zero. Inspired by the theoretical predictions, we have successfully fabricated a unique Ti3CNCl2@CoS2 core–shell nanostructure, which exhibits a significant enhancement in hydrogen evolution reaction (HER) activity.

Abstract

CoS2 is considered to be a promising electrocatalyst for hydrogen evolution reaction (HER). However, its further widespread applications are hampered by the unsatisfactory activity due to relatively high chemisorption energy for hydrogen atom. Herein, theoretical predictions of first-principles calculations reveal that the introduction of a Cl-terminated MXenes-Ti3CNCl2 can significantly reduce the HER potential of CoS2-based materials and the Ti3CNCl2@CoS2 core–shell nanostructure has Gibbs free energy of hydrogen adsorption (|ΔGH|) close to zero, much lower than that of the pristine CoS2 and Ti3CNCl2. Inspired by the theoretical predictions, we have successfully fabricated a unique Ti3CNCl2@CoS2 core–shell nanostructure by ingeniously coupling CoS2 with a Cl-terminated MXenes-Ti3CNCl2. Interface-charge transfer between CoS2 and Ti3CNCl2 results in a higher degree of electronic localization and a formation of chemical bonding. Thus, the Ti3CNCl2@CoS2 core–shell nanostructure achieves a significant enhancement in HER activity compared to pristine CoS2 and Ti3CNCl2. Theoretical calculations further confirm that the partial density of states of CoS2 after hybridization becomes more non-localized, and easier to interact with hydrogen ions, thus boosting HER performance. In this work, the success of oriented experimental fabrication of high-efficiency Ti3CNCl2@CoS2 electrocatalysts guided by theoretical predictions provides a powerful lead for the further strategic design and fabrication of efficient HER electrocatalysts.

Keywords

theoretical predictionsTi3CNCl2@CoS2 core–shell nanostructure electronic non-localizationhydrogen evolution

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Nano Research
Volume 15 Issue 7,
July 2022
Pages 5977-5986
DOI: 10.1007/s12274-022-4276-8
Cite this article:
Jiang J, Bai S, Yang M, et al. Strategic design and fabrication of MXenes-Ti3CNCl2@CoS2 core–shell nanostructure for high-efficiency hydrogen evolution. Nano Research, 2022, 15(7): 5977-5986. https://doi.org/10.1007/s12274-022-4276-8
Topics:
Electrocatalysis

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Received: 06 January 2022
Revised: 26 February 2022
Accepted: 27 February 2022
Published: 04 May 2022
© Tsinghua University Press 2022
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