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Title: Synergistic Phase and Disorder Engineering in 1T‐MoSe 2 Nanosheets for Enhanced Hydrogen‐Evolution Reaction

Abstract

MoSe 2 is a promising earth‐abundant electrocatalyst for the hydrogen‐evolution reaction (HER), even though it has received much less attention among the layered dichalcogenide (MX 2 ) materials than MoS 2 so far. Here, a novel hydrothermal‐synthesis strategy is presented to achieve simultaneous and synergistic modulation of crystal phase and disorder in partially crystallized 1T‐MoSe 2 nanosheets to dramatically enhance their HER catalytic activity. Careful structural characterization and defect characterization using positron annihilation lifetime spectroscopy correlated with electrochemical measurements show that the formation of the 1T phase under a large excess of the NaBH 4 reductant during synthesis can effectively improve the intrinsic activity and conductivity, and the disordered structure from a lower reaction temperature can provide abundant unsaturated defects as active sites. Such synergistic effects lead to superior HER catalytic activity with an overpotential of 152 mV versus reversible hydrogen electrode (RHE) for the electrocatalytic current density of j = −10 mA cm −2 , and a Tafel slope of 52 mV dec −1 . This work paves a new pathway for improving the catalytic activity of MoSe 2 and generally MX 2 ‐based electrocatalysts via a synergistic modulation strategy.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [3];  [4];  [5];  [6];  [6]; ORCiD logo [3]; ORCiD logo [7]
+ Show Author Affiliations
  1. Centre for Composite Materials and Structures Harbin Institute of Technology Harbin 150001 China
  2. Institute of Petrochemistry Heilongjiang Academy of Sciences Harbin 150040 China
  3. Academy of Fundamental and Interdisciplinary Sciences Department of Physics Harbin Institute of Technology Harbin 150001 China
  4. School of Materials Science and Engineering Dalian Jiaotong University Dalian 116028 China
  5. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 China
  6. Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China
  7. Department of Chemistry University of Wisconsin–Madison 1101 University Avenue Madison WI 53706 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1400842
Grant/Contract Number:  
DE‐FG02‐09ER46664
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Name: Advanced Materials Journal Volume: 29 Journal Issue: 28; Journal ID: ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Yin, Ying, Zhang, Yumin, Gao, Tangling, Yao, Tai, Zhang, Xinghong, Han, Jiecai, Wang, Xianjie, Zhang, Zhihua, Xu, Ping, Zhang, Peng, Cao, Xingzhong, Song, Bo, and Jin, Song. Synergistic Phase and Disorder Engineering in 1T‐MoSe 2 Nanosheets for Enhanced Hydrogen‐Evolution Reaction. Germany: N. p., 2017. Web. doi:10.1002/adma.201700311.
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Yin, Ying, Zhang, Yumin, Gao, Tangling, Yao, Tai, Zhang, Xinghong, Han, Jiecai, Wang, Xianjie, Zhang, Zhihua, Xu, Ping, Zhang, Peng, Cao, Xingzhong, Song, Bo, & Jin, Song. Synergistic Phase and Disorder Engineering in 1T‐MoSe 2 Nanosheets for Enhanced Hydrogen‐Evolution Reaction. Germany. https://doi.org/10.1002/adma.201700311
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Yin, Ying, Zhang, Yumin, Gao, Tangling, Yao, Tai, Zhang, Xinghong, Han, Jiecai, Wang, Xianjie, Zhang, Zhihua, Xu, Ping, Zhang, Peng, Cao, Xingzhong, Song, Bo, and Jin, Song. Fri . "Synergistic Phase and Disorder Engineering in 1T‐MoSe 2 Nanosheets for Enhanced Hydrogen‐Evolution Reaction". Germany. https://doi.org/10.1002/adma.201700311.
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@article{osti_1400842,
title = {Synergistic Phase and Disorder Engineering in 1T‐MoSe 2 Nanosheets for Enhanced Hydrogen‐Evolution Reaction},
author = {Yin, Ying and Zhang, Yumin and Gao, Tangling and Yao, Tai and Zhang, Xinghong and Han, Jiecai and Wang, Xianjie and Zhang, Zhihua and Xu, Ping and Zhang, Peng and Cao, Xingzhong and Song, Bo and Jin, Song},
abstractNote = {MoSe 2 is a promising earth‐abundant electrocatalyst for the hydrogen‐evolution reaction (HER), even though it has received much less attention among the layered dichalcogenide (MX 2 ) materials than MoS 2 so far. Here, a novel hydrothermal‐synthesis strategy is presented to achieve simultaneous and synergistic modulation of crystal phase and disorder in partially crystallized 1T‐MoSe 2 nanosheets to dramatically enhance their HER catalytic activity. Careful structural characterization and defect characterization using positron annihilation lifetime spectroscopy correlated with electrochemical measurements show that the formation of the 1T phase under a large excess of the NaBH 4 reductant during synthesis can effectively improve the intrinsic activity and conductivity, and the disordered structure from a lower reaction temperature can provide abundant unsaturated defects as active sites. Such synergistic effects lead to superior HER catalytic activity with an overpotential of 152 mV versus reversible hydrogen electrode (RHE) for the electrocatalytic current density of j = −10 mA cm −2 , and a Tafel slope of 52 mV dec −1 . This work paves a new pathway for improving the catalytic activity of MoSe 2 and generally MX 2 ‐based electrocatalysts via a synergistic modulation strategy.},
doi = {10.1002/adma.201700311},
journal = {Advanced Materials},
number = 28,
volume = 29,
place = {Germany},
year = {Fri May 19 00:00:00 EDT 2017},
month = {Fri May 19 00:00:00 EDT 2017}
}
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https://doi.org/10.1002/adma.201700311
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