Nanoscale mapping of hydrogen evolution on metallic and semiconducting MoS2 nanosheets
Abstract
Hydrogen evolution reaction (HER) on molybdenum disulfide (MoS2) nanosheets is enhanced for the metallic (1T) phase relative to the thermodynamically stable semiconducting (2H) phase. To measure this difference, we employ scanning electrochemical microscopy (SECM) for high-resolution mapping (<20 nm spatial resolution) of surface reactivity for mixed-phase and pure 2H-only MoS2 nanosheets. For mixed-phase MoS2 nanosheets, we find major differences in reactivity of the two phases for electron transfer involving ferrocenemethanol, allowing us to locate 1T and 2H regions and directly map the corresponding HER activity. In our measurements, we find that HER is immeasurably slow on the 2H basal plane and much faster on edges, whereas 1T portions are highly reactive across the entire portion. We also use scanning transmission electron microscopy-electron energy loss spectroscopy and scanning Kelvin probe microscopy to corroborate the phase domains and local workfunctions (surface potentials) within the MoS2 nanosheets; the mixed-phase MoS2 has a shallower workfunction compared to 2H MoS2, which could enable a greater driving force for H2 generation. As a result, this powerful combination of techniques for spatially mapping surface reactivity and correlated phase domains should be applicable to a broad range of materials for HER and other catalysis reactions.
- Authors:
-
- Queens College-CUNY, Flushing, NY (United States); Graduate Center of CUNY, New York, NY (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1524319
- Alternate Identifier(s):
- OSTI ID: 1484536
- Report Number(s):
- NREL/JA-5900-71993
Journal ID: ISSN 2055-6756; NHAOAW
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nanoscale Horizons
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 3; Journal ID: ISSN 2055-6756
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; electron energy levels; electron energy loss spectroscopy; electron scattering; energy dissipation; high resolution transmission electron microscopy; hydrogen; layered semiconductors; mapping; nanosheets; scanning; scanning electron microscopy; scanning probe microscopy; sulfur compounds
Citation Formats
Sun, Tong, Zhang, Hanyu, Wang, Xiang, Liu, Jun, Xiao, Chuanxiao, Nanayakkara, Sanjini U., Blackburn, Jeffrey L., Mirkin, Michael V., and Miller, Elisa M. Nanoscale mapping of hydrogen evolution on metallic and semiconducting MoS2 nanosheets. United States: N. p., 2018.
Web. doi:10.1039/C8NH00346G.
Sun, Tong, Zhang, Hanyu, Wang, Xiang, Liu, Jun, Xiao, Chuanxiao, Nanayakkara, Sanjini U., Blackburn, Jeffrey L., Mirkin, Michael V., & Miller, Elisa M. Nanoscale mapping of hydrogen evolution on metallic and semiconducting MoS2 nanosheets. United States. https://doi.org/10.1039/C8NH00346G
Sun, Tong, Zhang, Hanyu, Wang, Xiang, Liu, Jun, Xiao, Chuanxiao, Nanayakkara, Sanjini U., Blackburn, Jeffrey L., Mirkin, Michael V., and Miller, Elisa M. Thu .
"Nanoscale mapping of hydrogen evolution on metallic and semiconducting MoS2 nanosheets". United States. https://doi.org/10.1039/C8NH00346G. https://www.osti.gov/servlets/purl/1524319.
@article{osti_1524319,
title = {Nanoscale mapping of hydrogen evolution on metallic and semiconducting MoS2 nanosheets},
author = {Sun, Tong and Zhang, Hanyu and Wang, Xiang and Liu, Jun and Xiao, Chuanxiao and Nanayakkara, Sanjini U. and Blackburn, Jeffrey L. and Mirkin, Michael V. and Miller, Elisa M.},
abstractNote = {Hydrogen evolution reaction (HER) on molybdenum disulfide (MoS2) nanosheets is enhanced for the metallic (1T) phase relative to the thermodynamically stable semiconducting (2H) phase. To measure this difference, we employ scanning electrochemical microscopy (SECM) for high-resolution mapping (<20 nm spatial resolution) of surface reactivity for mixed-phase and pure 2H-only MoS2 nanosheets. For mixed-phase MoS2 nanosheets, we find major differences in reactivity of the two phases for electron transfer involving ferrocenemethanol, allowing us to locate 1T and 2H regions and directly map the corresponding HER activity. In our measurements, we find that HER is immeasurably slow on the 2H basal plane and much faster on edges, whereas 1T portions are highly reactive across the entire portion. We also use scanning transmission electron microscopy-electron energy loss spectroscopy and scanning Kelvin probe microscopy to corroborate the phase domains and local workfunctions (surface potentials) within the MoS2 nanosheets; the mixed-phase MoS2 has a shallower workfunction compared to 2H MoS2, which could enable a greater driving force for H2 generation. As a result, this powerful combination of techniques for spatially mapping surface reactivity and correlated phase domains should be applicable to a broad range of materials for HER and other catalysis reactions.},
doi = {10.1039/C8NH00346G},
journal = {Nanoscale Horizons},
number = 3,
volume = 4,
place = {United States},
year = {Thu Nov 29 00:00:00 EST 2018},
month = {Thu Nov 29 00:00:00 EST 2018}
}
Web of Science
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Works referencing / citing this record:
High‐Resolution Electrochemical Mapping of the Hydrogen Evolution Reaction on Transition‐Metal Dichalcogenide Nanosheets
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