Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies
Abstract
As a promising non-precious catalyst for the hydrogen evolution reaction, molybdenum disulphide (MoS2) is known to contain active edge sites and an inert basal plane. Activating the MoS2 basal plane could further enhance its HER activity but is not often a strategy for doing so. Herein, we report the first activation and optimization of the basal plane of monolayer 2H-MoS2 for HER by introducing sulphur (S) vacancies and strain. Our theoretical and experimental results show that the S-vacancies are new catalytic sites in the basal plane, where gap states around the Fermi level allow hydrogen to bind directly to exposed Mo atoms. The hydrogen adsorption free energy (ΔGH) can be further manipulated by straining the surface with S-vacancies, which fine-tunes the catalytic activity. Furthermore, proper combinations of S-vacancy and strain yield the optimal ΔGH = 0 eV, which allows us to achieve the highest intrinsic HER activity among molybdenum-sulphide-based catalysts.
- Authors:
-
- Stanford Univ., Stanford, CA (United States)
- Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center on Nanostructuring for Efficient Energy Conversion (CNEEC); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1257223
- Grant/Contract Number:
- AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 1; Journal ID: ISSN 1476-1122
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemical engineering; electrocatalysis; two-dimensional materials
Citation Formats
Li, Hong, Tsai, Charlie, Koh, Ai Leen, Cai, Lili, Contryman, Alex W., Fragapane, Alex H., Zhao, Jiheng, Han, Hyun Soon, Manoharan, Hari C., Abild-Pedersen, Frank, Nørskov, Jens K., and Zheng, Xiaolin. Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies. United States: N. p., 2015.
Web. doi:10.1038/NMAT4465.
Li, Hong, Tsai, Charlie, Koh, Ai Leen, Cai, Lili, Contryman, Alex W., Fragapane, Alex H., Zhao, Jiheng, Han, Hyun Soon, Manoharan, Hari C., Abild-Pedersen, Frank, Nørskov, Jens K., & Zheng, Xiaolin. Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies. United States. doi:https://doi.org/10.1038/NMAT4465
Li, Hong, Tsai, Charlie, Koh, Ai Leen, Cai, Lili, Contryman, Alex W., Fragapane, Alex H., Zhao, Jiheng, Han, Hyun Soon, Manoharan, Hari C., Abild-Pedersen, Frank, Nørskov, Jens K., and Zheng, Xiaolin. Mon .
"Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies". United States. doi:https://doi.org/10.1038/NMAT4465. https://www.osti.gov/servlets/purl/1257223.
@article{osti_1257223,
title = {Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies},
author = {Li, Hong and Tsai, Charlie and Koh, Ai Leen and Cai, Lili and Contryman, Alex W. and Fragapane, Alex H. and Zhao, Jiheng and Han, Hyun Soon and Manoharan, Hari C. and Abild-Pedersen, Frank and Nørskov, Jens K. and Zheng, Xiaolin},
abstractNote = {As a promising non-precious catalyst for the hydrogen evolution reaction, molybdenum disulphide (MoS2) is known to contain active edge sites and an inert basal plane. Activating the MoS2 basal plane could further enhance its HER activity but is not often a strategy for doing so. Herein, we report the first activation and optimization of the basal plane of monolayer 2H-MoS2 for HER by introducing sulphur (S) vacancies and strain. Our theoretical and experimental results show that the S-vacancies are new catalytic sites in the basal plane, where gap states around the Fermi level allow hydrogen to bind directly to exposed Mo atoms. The hydrogen adsorption free energy (ΔGH) can be further manipulated by straining the surface with S-vacancies, which fine-tunes the catalytic activity. Furthermore, proper combinations of S-vacancy and strain yield the optimal ΔGH = 0 eV, which allows us to achieve the highest intrinsic HER activity among molybdenum-sulphide-based catalysts.},
doi = {10.1038/NMAT4465},
journal = {Nature Materials},
number = 1,
volume = 15,
place = {United States},
year = {2015},
month = {11}
}
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