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Title: Electrochemical generation of sulfur vacancies in the basal plane of MoS2 for hydrogen evolution

Abstract

Recently, sulfur (S)-vacancies created on the basal plane of 2H-molybdenum disulfide (MoS 2) using argon plasma exposure exhibited higher intrinsic activity for the electrochemical hydrogen evolution reaction than the edge sites and metallic 1T-phase of MoS 2 catalysts. But, a more industrially viable alternative to the argon plasma desulfurization process is needed. In this work, we introduce a scalable route towards generating S-vacancies on the MoS 2 basal plane using electrochemical desulfurization. We found that they can be electrochemically reduced under accessible applied potentials, even though sulfur atoms on the basal plane are known to be stable and inert. This can be done on various 2H-MoS 2 nanostructures. Furthermore, by changing the applied desulfurization potential, the extent of desulfurization and the resulting activity can be varied. The resulting active sites are stable under extended desulfurization durations and show consistent HER activity.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [3];  [1];  [3];  [1]
  1. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis; SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
  2. Stanford Univ., CA (United States). Dept. of Mechanical Engineering; Nanyang Technological Univ. (Singapore). School of Mechanical and Aerospace Engineering
  3. Stanford Univ., CA (United States). Dept. of Mechanical Engineering
  4. Stanford Univ., CA (United States). Dept. of Material Science and Engineering
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1360913
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
70 PLASMA PHYSICS AND FUSION TECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemical engineering; electrocatalysis; hydrogen fuel

Citation Formats

Tsai, Charlie, Li, Hong, Park, Sangwook, Park, Joonsuk, Han, Hyun Soo, Nørskov, Jens K., Zheng, Xiaolin, and Abild-Pedersen, Frank. Electrochemical generation of sulfur vacancies in the basal plane of MoS2 for hydrogen evolution. United States: N. p., 2017. Web. doi:10.1038/ncomms15113.
Tsai, Charlie, Li, Hong, Park, Sangwook, Park, Joonsuk, Han, Hyun Soo, Nørskov, Jens K., Zheng, Xiaolin, & Abild-Pedersen, Frank. Electrochemical generation of sulfur vacancies in the basal plane of MoS2 for hydrogen evolution. United States. doi:10.1038/ncomms15113.
Tsai, Charlie, Li, Hong, Park, Sangwook, Park, Joonsuk, Han, Hyun Soo, Nørskov, Jens K., Zheng, Xiaolin, and Abild-Pedersen, Frank. Fri . "Electrochemical generation of sulfur vacancies in the basal plane of MoS2 for hydrogen evolution". United States. doi:10.1038/ncomms15113. https://www.osti.gov/servlets/purl/1360913.
@article{osti_1360913,
title = {Electrochemical generation of sulfur vacancies in the basal plane of MoS2 for hydrogen evolution},
author = {Tsai, Charlie and Li, Hong and Park, Sangwook and Park, Joonsuk and Han, Hyun Soo and Nørskov, Jens K. and Zheng, Xiaolin and Abild-Pedersen, Frank},
abstractNote = {Recently, sulfur (S)-vacancies created on the basal plane of 2H-molybdenum disulfide (MoS2) using argon plasma exposure exhibited higher intrinsic activity for the electrochemical hydrogen evolution reaction than the edge sites and metallic 1T-phase of MoS2 catalysts. But, a more industrially viable alternative to the argon plasma desulfurization process is needed. In this work, we introduce a scalable route towards generating S-vacancies on the MoS2 basal plane using electrochemical desulfurization. We found that they can be electrochemically reduced under accessible applied potentials, even though sulfur atoms on the basal plane are known to be stable and inert. This can be done on various 2H-MoS2 nanostructures. Furthermore, by changing the applied desulfurization potential, the extent of desulfurization and the resulting activity can be varied. The resulting active sites are stable under extended desulfurization durations and show consistent HER activity.},
doi = {10.1038/ncomms15113},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {Fri Apr 21 00:00:00 EDT 2017},
month = {Fri Apr 21 00:00:00 EDT 2017}
}

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Cited by: 15 works
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