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Title: Rational design of stable sulfur vacancies in molybdenum disulfide for hydrogen evolution

Abstract

Sulfur (S) vacancies in MoS2 have been found to act as a new active center, which shows an unprecedented intrinsic HER activity under elastic strain. However, such S-vacancies are unstable and the activities are very sensitive to the vacancy concentration. A strategy to stabilize these abundant active sites is thus highly desirable. Herein, we rationally design a catalyst system to stabilize S-vacancies in the basal plane of $2H-$MoS2 supported on defective vertical graphene network (VGN). The energetically favorable line-shaped S-vacancies in MoS2 shows a consistently high HER activity that is insensitive to S-vacancy concentration. Moreover, the defective graphene support effectively stabilizes these S-vacancies. The optimized catalyst exhibits a superior HER activity with overpotential of 128 mV at 10 mA cm-2 and Tafel slope of 50 mV dec-1. Most importantly, the catalyst shows greatly increased stability over 500 h; benchmarking the most stable nonprecious HER catalyst in acidic media to date.

Authors:
 [1];  [2];  [3];  [3]; ORCiD logo [4];  [5];  [6]; ORCiD logo [7]
  1. Nanyang Technological Univ. (Singapore); Chinese Academy of Sciences (CAS), Ningbo (China)
  2. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis
  3. Chinese Academy of Sciences (CAS), Ningbo (China)
  4. CSIRO Manufacturing, Lindfield, NSW (Australia); Univ. of New South Wales, Sydney, NSW (Australia)
  5. Technical Univ. of Denmark, Lyngby (Denmark)
  6. Sun Yat-Sen Univ., Guangzhou (China)
  7. Nanyang Technological Univ. (Singapore)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1580683
Alternate Identifier(s):
OSTI ID: 1591954
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 382; Journal Issue: C; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 2D heterostructure; hydrogen evolution; stabilization function; vacancies; long-term stability

Citation Formats

Zhao, Yunxing, Tang, Michael T., Wu, Sudong, Geng, Jing, Han, Zhaojun, Chan, Karen, Gao, Pingqi, and Li, Hong. Rational design of stable sulfur vacancies in molybdenum disulfide for hydrogen evolution. United States: N. p., 2020. Web. https://doi.org/10.1016/j.jcat.2019.12.028.
Zhao, Yunxing, Tang, Michael T., Wu, Sudong, Geng, Jing, Han, Zhaojun, Chan, Karen, Gao, Pingqi, & Li, Hong. Rational design of stable sulfur vacancies in molybdenum disulfide for hydrogen evolution. United States. https://doi.org/10.1016/j.jcat.2019.12.028
Zhao, Yunxing, Tang, Michael T., Wu, Sudong, Geng, Jing, Han, Zhaojun, Chan, Karen, Gao, Pingqi, and Li, Hong. Sat . "Rational design of stable sulfur vacancies in molybdenum disulfide for hydrogen evolution". United States. https://doi.org/10.1016/j.jcat.2019.12.028. https://www.osti.gov/servlets/purl/1580683.
@article{osti_1580683,
title = {Rational design of stable sulfur vacancies in molybdenum disulfide for hydrogen evolution},
author = {Zhao, Yunxing and Tang, Michael T. and Wu, Sudong and Geng, Jing and Han, Zhaojun and Chan, Karen and Gao, Pingqi and Li, Hong},
abstractNote = {Sulfur (S) vacancies in MoS2 have been found to act as a new active center, which shows an unprecedented intrinsic HER activity under elastic strain. However, such S-vacancies are unstable and the activities are very sensitive to the vacancy concentration. A strategy to stabilize these abundant active sites is thus highly desirable. Herein, we rationally design a catalyst system to stabilize S-vacancies in the basal plane of $2H-$MoS2 supported on defective vertical graphene network (VGN). The energetically favorable line-shaped S-vacancies in MoS2 shows a consistently high HER activity that is insensitive to S-vacancy concentration. Moreover, the defective graphene support effectively stabilizes these S-vacancies. The optimized catalyst exhibits a superior HER activity with overpotential of 128 mV at 10 mA cm-2 and Tafel slope of 50 mV dec-1. Most importantly, the catalyst shows greatly increased stability over 500 h; benchmarking the most stable nonprecious HER catalyst in acidic media to date.},
doi = {10.1016/j.jcat.2019.12.028},
journal = {Journal of Catalysis},
number = C,
volume = 382,
place = {United States},
year = {2020},
month = {2}
}

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Cited by: 4 works
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