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Title: Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS2/WTe2 Hybrid Structures

Abstract

Using the MoS2–WTe2 heterostructure as a model system combined with electrochemical microreactors and density function theory calculations, it is shown that heterostructured contacts enhance the hydrogen evolution reaction (HER) activity of monolayer MoS2. Two possible mechanisms are suggested to explain this enhancement: efficient charge injection through large–area heterojunctions between MoS2 and WTe2 and effective screening of mirror charges due to the semimetallic nature of WTe2. The dielectric screening effect is proven minor, probed by measuring the HER activity of monolayer MoS2 on various support substrates with dielectric constants ranging from 4 to 300. Thus, the enhanced HER is attributed to the increased charge injection into MoS2 through large–area heterojunctions. Based on this understanding, a MoS2/WTe2 hybrid catalyst is fabricated with an HER overpotential of –140 mV at 10 mA cm–2, a Tafel slope of 40 mV dec–1, and long stability. Furthermore, these results demonstrate the importance of interfacial design in transition metal dichalcogenide HER catalysts. The microreactor platform presents an unambiguous approach to probe interfacial effects in various electrocatalytic reactions.

Authors:
 [1];  [1];  [2];  [1];  [1];  [3];  [4];  [5];  [6];  [7];  [8];  [2];  [4];  [4];  [7];  [4];  [4];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Yale Univ., New Haven, CT (United States); Yale West Campus, West Haven, CT (United States)
  2. Uppsala Univ., Uppsala (Sweden)
  3. North Carolina State Univ., Raleigh, NC (United States)
  4. Yale West Campus, West Haven, CT (United States); Yale Univ., New Haven, CT (United States)
  5. Northwestern Polytechnical Univ., Xi'an (People's Republic of China)
  6. Yale Univ., New Haven, CT (United States)
  7. Tsinghua Univ., Beijing (People's Republic of China)
  8. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1558253
Report Number(s):
BNL-212011-2019-JAAM
Journal ID: ISSN 1613-6810
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Volume: 15; Journal Issue: 19; Journal ID: ISSN 1613-6810
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; electrochemical microreactors; heterostructures; hydrogen evolution reaction; interfacial effects; MoS2/WTe2 hybrid

Citation Formats

Zhou, Yu, Pondick, Joshua V., Silva, Jose Luis, Woods, John M., Hynek, David J., Matthews, Grace, Shen, Xin, Feng, Qingliang, Liu, Wen, Lu, Zhixing, Liang, Zhixiu, Brena, Barbara, Cai, Zhao, Wu, Min, Jiao, Liying, Hu, Shu, Wang, Hailiang, Araujo, Carlos Moyses, and Cha, Judy J. Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS2/WTe2 Hybrid Structures. United States: N. p., 2019. Web. doi:10.1002/smll.201900078.
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Zhou, Yu, Pondick, Joshua V., Silva, Jose Luis, Woods, John M., Hynek, David J., Matthews, Grace, Shen, Xin, Feng, Qingliang, Liu, Wen, Lu, Zhixing, Liang, Zhixiu, Brena, Barbara, Cai, Zhao, Wu, Min, Jiao, Liying, Hu, Shu, Wang, Hailiang, Araujo, Carlos Moyses, & Cha, Judy J. Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS2/WTe2 Hybrid Structures. United States. https://doi.org/10.1002/smll.201900078
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Zhou, Yu, Pondick, Joshua V., Silva, Jose Luis, Woods, John M., Hynek, David J., Matthews, Grace, Shen, Xin, Feng, Qingliang, Liu, Wen, Lu, Zhixing, Liang, Zhixiu, Brena, Barbara, Cai, Zhao, Wu, Min, Jiao, Liying, Hu, Shu, Wang, Hailiang, Araujo, Carlos Moyses, and Cha, Judy J. Mon . "Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS2/WTe2 Hybrid Structures". United States. https://doi.org/10.1002/smll.201900078. https://www.osti.gov/servlets/purl/1558253.
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@article{osti_1558253,
title = {Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS2/WTe2 Hybrid Structures},
author = {Zhou, Yu and Pondick, Joshua V. and Silva, Jose Luis and Woods, John M. and Hynek, David J. and Matthews, Grace and Shen, Xin and Feng, Qingliang and Liu, Wen and Lu, Zhixing and Liang, Zhixiu and Brena, Barbara and Cai, Zhao and Wu, Min and Jiao, Liying and Hu, Shu and Wang, Hailiang and Araujo, Carlos Moyses and Cha, Judy J.},
abstractNote = {Using the MoS2–WTe2 heterostructure as a model system combined with electrochemical microreactors and density function theory calculations, it is shown that heterostructured contacts enhance the hydrogen evolution reaction (HER) activity of monolayer MoS2. Two possible mechanisms are suggested to explain this enhancement: efficient charge injection through large–area heterojunctions between MoS2 and WTe2 and effective screening of mirror charges due to the semimetallic nature of WTe2. The dielectric screening effect is proven minor, probed by measuring the HER activity of monolayer MoS2 on various support substrates with dielectric constants ranging from 4 to 300. Thus, the enhanced HER is attributed to the increased charge injection into MoS2 through large–area heterojunctions. Based on this understanding, a MoS2/WTe2 hybrid catalyst is fabricated with an HER overpotential of –140 mV at 10 mA cm–2, a Tafel slope of 40 mV dec–1, and long stability. Furthermore, these results demonstrate the importance of interfacial design in transition metal dichalcogenide HER catalysts. The microreactor platform presents an unambiguous approach to probe interfacial effects in various electrocatalytic reactions.},
doi = {10.1002/smll.201900078},
journal = {Small},
number = 19,
volume = 15,
place = {United States},
year = {Mon Apr 08 00:00:00 EDT 2019},
month = {Mon Apr 08 00:00:00 EDT 2019}
}
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https://doi.org/10.1002/smll.201900078
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    Works referencing / citing this record:

    Tunable doping of N and S in carbon nanotubes by retarding pyrolysis-gas diffusion to promote electrocatalytic hydrogen evolution
    journal, January 2019

    • Wu, Hao; Chen, Zhimin; Xiao, Fei
    • Chemical Communications, Vol. 55, Issue 67
    • DOI: 10.1039/c9cc04869c

    Hydrogen evolution activity tuning via two-dimensional electron accumulation at buried interfaces
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    • Xue, Yudong; Fishman, Zachary S.; Wang, Yunting
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    • DOI: 10.1039/c9ta07123g
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