All the catalytic active sites of MoS2 for hydrogen evolution
Abstract
MoS2 presents a promising low-cost catalyst for the hydrogen evolution reaction (HER), but the understanding about its active sites has remained limited. Here we present an unambiguous study of the catalytic activities of all possible reaction sites of MoS2, including edge sites, sulfur vacancies, and grain boundaries. We demonstrate that, in addition to the well-known catalytically active edge sites, sulfur vacancies provide another major active site for the HER, while the catalytic activity of grain boundaries is much weaker. Here, the intrinsic turnover frequencies (Tafel slopes) of the edge sites, sulfur vacancies, and grain boundaries are estimated to be 7.5 s–1 (65–75 mV/dec), 3.2 s–1 (65–85 mV/dec), and 0.1 s–1 (120–160 mV/dec), respectively. We also demonstrate that the catalytic activity of sulfur vacancies strongly depends on the density of the vacancies and the local crystalline structure in proximity to the vacancies. Unlike edge sites, whose catalytic activity linearly depends on the length, sulfur vacancies show optimal catalytic activities when the vacancy density is in the range of 7–10%, and the number of sulfur vacancies in high crystalline quality MoS2 is higher than that in low crystalline quality MoS2, which may be related with the proximity of different local crystalline structuresmore »
- Authors:
-
[3];
[1];
[1];
[1]
- North Carolina State Univ., Raleigh, NC (United States)
- Duke Univ., Durham, NC (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1347369
- Report Number(s):
- BNL-113649-2017-JA
Journal ID: ISSN 0002-7863; R&D Project: MA015MACA; KC0201010
- Grant/Contract Number:
- SC00112704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 138; Journal Issue: 51; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Li, Guoqing, Zhang, Du, Qiao, Qiao, Yu, Yifei, Peterson, David, Zafar, Abdullah, Kumar, Raj, Curtarolo, Stefano, Hunte, Frank, Shannon, Steve, Zhu, Yimei, Yang, Weitao, and Cao, Linyou. All the catalytic active sites of MoS2 for hydrogen evolution. United States: N. p., 2016.
Web. doi:10.1021/jacs.6b05940.
Li, Guoqing, Zhang, Du, Qiao, Qiao, Yu, Yifei, Peterson, David, Zafar, Abdullah, Kumar, Raj, Curtarolo, Stefano, Hunte, Frank, Shannon, Steve, Zhu, Yimei, Yang, Weitao, & Cao, Linyou. All the catalytic active sites of MoS2 for hydrogen evolution. United States. https://doi.org/10.1021/jacs.6b05940
Li, Guoqing, Zhang, Du, Qiao, Qiao, Yu, Yifei, Peterson, David, Zafar, Abdullah, Kumar, Raj, Curtarolo, Stefano, Hunte, Frank, Shannon, Steve, Zhu, Yimei, Yang, Weitao, and Cao, Linyou. Tue .
"All the catalytic active sites of MoS2 for hydrogen evolution". United States. https://doi.org/10.1021/jacs.6b05940. https://www.osti.gov/servlets/purl/1347369.
@article{osti_1347369,
title = {All the catalytic active sites of MoS2 for hydrogen evolution},
author = {Li, Guoqing and Zhang, Du and Qiao, Qiao and Yu, Yifei and Peterson, David and Zafar, Abdullah and Kumar, Raj and Curtarolo, Stefano and Hunte, Frank and Shannon, Steve and Zhu, Yimei and Yang, Weitao and Cao, Linyou},
abstractNote = {MoS2 presents a promising low-cost catalyst for the hydrogen evolution reaction (HER), but the understanding about its active sites has remained limited. Here we present an unambiguous study of the catalytic activities of all possible reaction sites of MoS2, including edge sites, sulfur vacancies, and grain boundaries. We demonstrate that, in addition to the well-known catalytically active edge sites, sulfur vacancies provide another major active site for the HER, while the catalytic activity of grain boundaries is much weaker. Here, the intrinsic turnover frequencies (Tafel slopes) of the edge sites, sulfur vacancies, and grain boundaries are estimated to be 7.5 s–1 (65–75 mV/dec), 3.2 s–1 (65–85 mV/dec), and 0.1 s–1 (120–160 mV/dec), respectively. We also demonstrate that the catalytic activity of sulfur vacancies strongly depends on the density of the vacancies and the local crystalline structure in proximity to the vacancies. Unlike edge sites, whose catalytic activity linearly depends on the length, sulfur vacancies show optimal catalytic activities when the vacancy density is in the range of 7–10%, and the number of sulfur vacancies in high crystalline quality MoS2 is higher than that in low crystalline quality MoS2, which may be related with the proximity of different local crystalline structures to the vacancies.},
doi = {10.1021/jacs.6b05940},
journal = {Journal of the American Chemical Society},
number = 51,
volume = 138,
place = {United States},
year = {Tue Nov 29 00:00:00 EST 2016},
month = {Tue Nov 29 00:00:00 EST 2016}
}
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