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Title: Engineering Substrate Interaction To Improve Hydrogen Evolution Catalysis of Monolayer MoS2 Films beyond Pt

Abstract

MoS2 holds great promise as a cost-effective alternative to Pt for catalyzing the hydrogen evolution reaction (HER) of water, but its reported catalytic efficiency is still worse than that of Pt, the best HER catalyst but too rare and expensive for mass production of hydrogen. Here, we report a strategy to enable the catalytic activity of monolayer MoS2 films that are even better than that of Pt via engineering the interaction of the monolayer with supporting substrates. The monolayer films were grown with chemical vapor deposition processes and controlled to have an optimal density (7–10%) of sulfur vacancies. We find that the catalytic activity of MoS2 can be affected by substrates in two ways: forming an interfacial tunneling barrier with MoS2 and modifying the chemical nature of MoS2via charge transfer (proximity doping). Following this understanding, we enable excellent catalytic activities at the monolayer MoS2 films by using substrates that can provide n-doping to MoS2 and form low interfacial tunneling barriers with MoS2, such as Ti. The catalytic performance may be further boosted to be even better than Pt by crumpling the films on Ti coated flexible polymer substrates, as the Tafel slope of the film is substantially decreased with themore » presence of crumpling-induced compressive strain. The monolayer MoS2 films show no degradation in catalytic performance after being continuously tested for over 2 months.« less

Authors:
 [1];  [2];  [3];  [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
  1. North Carolina State Univ., Raleigh, NC (United States)
  2. Duke Univ., Durham, NC (United States)
  3. Univ. of Texas, Austin, TX (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Temple Univ., Philadelphia, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Welch Foundations
OSTI Identifier:
1608110
Grant/Contract Number:  
SC0012575; 1900039; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 14; Journal Issue: 2; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; MoS2; hydrogen evolution reaction; water splitting; 2D materials; substrate effects

Citation Formats

Li, Guoqing, Chen, Zehua, Li, Yifan, Zhang, Du, Yang, Weitao, Liu, Yuanyue, and Cao, Linyou. Engineering Substrate Interaction To Improve Hydrogen Evolution Catalysis of Monolayer MoS2 Films beyond Pt. United States: N. p., 2020. Web. https://doi.org/10.1021/acsnano.9b07324.
Li, Guoqing, Chen, Zehua, Li, Yifan, Zhang, Du, Yang, Weitao, Liu, Yuanyue, & Cao, Linyou. Engineering Substrate Interaction To Improve Hydrogen Evolution Catalysis of Monolayer MoS2 Films beyond Pt. United States. https://doi.org/10.1021/acsnano.9b07324
Li, Guoqing, Chen, Zehua, Li, Yifan, Zhang, Du, Yang, Weitao, Liu, Yuanyue, and Cao, Linyou. Thu . "Engineering Substrate Interaction To Improve Hydrogen Evolution Catalysis of Monolayer MoS2 Films beyond Pt". United States. https://doi.org/10.1021/acsnano.9b07324. https://www.osti.gov/servlets/purl/1608110.
@article{osti_1608110,
title = {Engineering Substrate Interaction To Improve Hydrogen Evolution Catalysis of Monolayer MoS2 Films beyond Pt},
author = {Li, Guoqing and Chen, Zehua and Li, Yifan and Zhang, Du and Yang, Weitao and Liu, Yuanyue and Cao, Linyou},
abstractNote = {MoS2 holds great promise as a cost-effective alternative to Pt for catalyzing the hydrogen evolution reaction (HER) of water, but its reported catalytic efficiency is still worse than that of Pt, the best HER catalyst but too rare and expensive for mass production of hydrogen. Here, we report a strategy to enable the catalytic activity of monolayer MoS2 films that are even better than that of Pt via engineering the interaction of the monolayer with supporting substrates. The monolayer films were grown with chemical vapor deposition processes and controlled to have an optimal density (7–10%) of sulfur vacancies. We find that the catalytic activity of MoS2 can be affected by substrates in two ways: forming an interfacial tunneling barrier with MoS2 and modifying the chemical nature of MoS2via charge transfer (proximity doping). Following this understanding, we enable excellent catalytic activities at the monolayer MoS2 films by using substrates that can provide n-doping to MoS2 and form low interfacial tunneling barriers with MoS2, such as Ti. The catalytic performance may be further boosted to be even better than Pt by crumpling the films on Ti coated flexible polymer substrates, as the Tafel slope of the film is substantially decreased with the presence of crumpling-induced compressive strain. The monolayer MoS2 films show no degradation in catalytic performance after being continuously tested for over 2 months.},
doi = {10.1021/acsnano.9b07324},
journal = {ACS Nano},
number = 2,
volume = 14,
place = {United States},
year = {2020},
month = {1}
}

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