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Research Article

Rationally engineered Co and N co-doped WS2 as bifunctional catalysts for pH-universal hydrogen evolution and oxidative dehydrogenation reactions

Min Ling1,§, Na Li1,§, Binbin Jiang3,§, Renyong Tu4, Tao Wu1, Pingli Guan1, Yin Ye1, Weng-Chon (Max) Cheong4,5, Kaian Sun4, Shoujie Liu6, Konglin Wu1,2( ), Aijian Huang4,7( ), Xianwen Wei1,2( )
College of Chemistry and Materials Science, Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education Institutes, Key Laboratory of Functional Molecular Solids, the Ministry of Education, Anhui Normal University, Wuhu 241002, China
School of Chemistry and Chemical Engineering, Institute of Clean Energy and Advanced Nanocatalysis (iClean), Anhui Province Key Laboratory of Coal Clean Conversion and High Valued Utilization, Anhui University of Technology, Maanshan 243002, China
School of Chemistry and Chemical Engineering, Anhui Key Laboratory of Photoelectric-Magnetic Functional Materials, Anqing Normal University, Anqing 246011, China
Department of Chemistry, Tsinghua University, Beijing 100084, China
Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao, China
Chemistry and Chemical Engineering of Guangdong Laboratory, Shantou 515063, China
School of Electronics Science and Engineering, University of Electronic Science and Technology of China, Chengdu 610054, China

§Min Ling, Na Li, and Binbin Jiang contributed equally to this work.

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Graphical Abstract

Abstract

In the field of electrolysis of water, the design and synthesis of catalysts over a wide pH range have attracted extensive attentions. In this paper, Co and N are co-introduced into the structural unit of tungsten disulfide (WS2), and the hydrogen evolution reaction (HER) performances of different WS2-based catalysts are theoretically predicted and systematically studied by density functional theory (DFT) calculations. With the guidance of DFT calculations, an evaporation-pyrolysis strategy is applied to prepare Co and N co-doped WS2 (Co,N-WS2) flower-like nanosheets, which exhibits excellent HER performance over a wide pH range. In addition, the DFT calculations show that the active sites in Co,N-WS2 have a good ability of hydrogen adsorption after the introduction of Co and N, suggesting that such a co-doping system will be an ideal catalyst for oxidative dehydrogenation (ODH). The following experiment results indeed evidence that the Co,N-WS2 catalyst displays a high activity in the ODH of 1,2,3,4-tetrahydroquinoline (4H-quinoline) and its derivatives. Therefore, this work provides a good example for the rational design and accurate preparation of functional catalysts, which enables it possible to develop other efficient catalysts with multiple functions.

Keywords

WS2heteroatomic dopingbifunctional catalystdensity functional theory (DFT) calculationelectrolysis of water

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Nano Research
Volume 15 Issue 3,
March 2022
Pages 1993-2002
DOI: 10.1007/s12274-021-3898-6
Cite this article:
Ling M, Li N, Jiang B, et al. Rationally engineered Co and N co-doped WS2 as bifunctional catalysts for pH-universal hydrogen evolution and oxidative dehydrogenation reactions. Nano Research, 2022, 15(3): 1993-2002. https://doi.org/10.1007/s12274-021-3898-6
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Received: 10 August 2021
Revised: 02 September 2021
Accepted: 18 September 2021
Published: 09 November 2021
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021
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