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Nano Research 2023, 16(5): 6228-6236 https://doi.org/10.1007/s12274-022-5287-1
Research Article | Issue | Published: 14 December 2022

P-band center theory guided activation of MoS2 basal S sites for pH-universal hydrogen evolution

Show Author's Information Chao Meng1,2,  Yuanfeng Gao3,  Yue Zhou3( ),  Kang Sun4,  Yanmin Wang3,  Ye Han5( ),  Qianqian Zhao2,  Xuemin Chen6,  Han Hu1( ),  Mingbo Wu1
State Key Laboratory of Heavy Oil Processing, Institute of New Energy, China University of Petroleum (East China), Qingdao 266580, China
College of Electrical Engineering and Automation, Shandong University of Science and Technology, Qingdao 266590, China
College of Energy Storage Technology, Shandong University of Science and Technology, Qingdao 266590, China
Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry, Nanjing 210042, China
School of Materials Science and Engineering, Shandong University of Science and Technology, Qingdao 266590, China
College of Science, Hebei University of Science and Technology, Shijiazhuang 050018, China
Keywords:
molybdenum disulfide, hydrogen evolution, p-orbital electron structure, basal S sites, synergistic mechanism
Topics:
Hydrogen evolution reaction
Cite this article:
Meng C, Gao Y, Zhou Y, et al. P-band center theory guided activation of MoS2 basal S sites for pH-universal hydrogen evolution. Nano Research, 2023, 16(5): 6228-6236. https://doi.org/10.1007/s12274-022-5287-1
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Abstract Full text Electronic supplementary material About this article

The edge S sites of thermodynamically stable 2H MoS2 are active for hydrogen evolution reaction (HER) but the active sites are scarce. Despite the dominance of the basal S sites, they are generally inert to HER because of the low p-band center. Herein, we reported a synergistic combination of phase engineering and NH4+ intercalation to promote the HER performance of MoS2. The rational combination of 1T and 2H phases raises the p-band center of the basal S sites while the intercalated NH4+ ions further optimize and stabilize the electronic band of these sites. The S sites with regulated band structures afford moderate hydrogen adsorption, thus contributing to excellent HER performance over a wide pH range. In an acid medium, this catalyst exhibits a low overpotential of 169 mV at 10 mA·cm−2 and Tafel slope of 39 mV·dec−1 with robust stability, superior to most of recently reported MoS2-based non-noble catalysts. The combined use of in/ex-situ characterizations ravels that the appearance of more unpaired electrons at the Mo 4d-orbital reduces the d-band center which upshifts the p-band center of the adjacent S for essentially improved HER performance. This work provides guidelines for the future development of layered transition-metal-dichalcogenide catalysts.


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About this article

P-band center theory guided activation of MoS2 basal S sites for pH-universal hydrogen evolution

Show Author's information Chao Meng1,2, Yuanfeng Gao3, Yue Zhou3( ), Kang Sun4, Yanmin Wang3, Ye Han5( ), Qianqian Zhao2, Xuemin Chen6, Han Hu1( ), Mingbo Wu1
State Key Laboratory of Heavy Oil Processing, Institute of New Energy, China University of Petroleum (East China), Qingdao 266580, China
College of Electrical Engineering and Automation, Shandong University of Science and Technology, Qingdao 266590, China
College of Energy Storage Technology, Shandong University of Science and Technology, Qingdao 266590, China
Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry, Nanjing 210042, China
School of Materials Science and Engineering, Shandong University of Science and Technology, Qingdao 266590, China
College of Science, Hebei University of Science and Technology, Shijiazhuang 050018, China

Abstract

The edge S sites of thermodynamically stable 2H MoS2 are active for hydrogen evolution reaction (HER) but the active sites are scarce. Despite the dominance of the basal S sites, they are generally inert to HER because of the low p-band center. Herein, we reported a synergistic combination of phase engineering and NH4+ intercalation to promote the HER performance of MoS2. The rational combination of 1T and 2H phases raises the p-band center of the basal S sites while the intercalated NH4+ ions further optimize and stabilize the electronic band of these sites. The S sites with regulated band structures afford moderate hydrogen adsorption, thus contributing to excellent HER performance over a wide pH range. In an acid medium, this catalyst exhibits a low overpotential of 169 mV at 10 mA·cm−2 and Tafel slope of 39 mV·dec−1 with robust stability, superior to most of recently reported MoS2-based non-noble catalysts. The combined use of in/ex-situ characterizations ravels that the appearance of more unpaired electrons at the Mo 4d-orbital reduces the d-band center which upshifts the p-band center of the adjacent S for essentially improved HER performance. This work provides guidelines for the future development of layered transition-metal-dichalcogenide catalysts.

Keywords: molybdenum disulfide, hydrogen evolution, p-orbital electron structure, basal S sites, synergistic mechanism

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Publication history
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Acknowledgements

Publication history

Received: 11 September 2022
Revised: 27 October 2022
Accepted: 31 October 2022
Published: 14 December 2022
Issue date: May 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 51901115 and 51802075), the Shandong Provincial Natural Science Foundation, China (Nos. ZR2019PEM001, ZR2019BB009, and ZR2020ZD08), and the Young Talents Program in University of Hebei Province, China (No. BJ2019002).

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