The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen
Abstract
The excellent catalytic activity of metallic MoS2 edges for the hydrogen evolution reaction (HER) has led to substantial efforts towards increasing the edge concentration. The 2H basal plane is less active for the HER because it is less conducting and therefore possesses less efficient charge transfer kinetics. Here we show that the activity of the 2H basal planes of monolayer MoS2 nanosheets can be made comparable to state-of-the-art catalytic properties of metallic edges and the 1T phase by improving the electrical coupling between the substrate and the catalyst so that electron injection from the electrode and transport to the catalyst active site is facilitated. Phase-engineered low-resistance contacts on monolayer 2H-phase MoS2 basal plane lead to higher efficiency of charge injection in the nanosheets so that its intrinsic activity towards the HER can be measured. We demonstrate that onset potentials and Tafel slopes of ∼-0.1 V and ∼50 mV per decade can be achieved from 2H-phase catalysts where only the basal plane is exposed. We show that efficient charge injection and the presence of naturally occurring sulfur vacancies are responsible for the observed increase in catalytic activity of the 2H basal plane. Our results provide new insights into the role of contact resistance and charge transport on the performance of two-dimensional MoS2 nanosheet catalysts for the HER.
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The HER overpotential values of Fe/GD and Ni/GD are superior to other earth-abundant HER electrocatalysts such as Ni2P, MoS2, and exfoliated WS2, and compare favorably with noble-metal-based electrocatalysts such as Pt nanowires/single-layered Ni(OH)2.
“The values are superior to other earth-abundant HER electrocatalysts [such as Ni2P (~110 mA cm–2)43, MoS2 (170 mA cm–2)44, and exfoliated WS2 (210 mA cm–2)45], and even compare favorably with noble-metal-based electrocatalysts such as Pt nanowires/single-layered Ni(OH)246.”
From Anchoring zero valence single atoms of nickel and iron on graphdiyne for hydrogen evolution (2018) · cites this paper as [44]
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- Authors
- Voiry, D., Fullon, R., Yang, J., de Carvalho Castro e Silva, C., Kappera, R., Bozkurt, I., Kaplan, D., Lagos, M. J., Batson, P. E., Gupta, G., Mohite, A. D., Dong, L., Er, D., Shenoy, V. B., Asefa, T., & Chhowalla, M.
- Affiliations
- Rutgers, The State University of New Jersey (US)
- United States Department of the Army (US)
- Los Alamos National Laboratory (US)
- University of Pennsylvania (US)
- Corresponding author
- Chhowalla, Manish
- ORCID
- Venue
- Nature Materials
- Published
- 2016-06-13
- Volume
- 15
- Issue
- 9
- Pages
- 1003-1009
- ISSN
- 1476-1122 (ISSN-L)
- 1476-4660
- OpenAlex
- W2432559505
- Cited by
- 824
- References
- 8
- Citations by year
- 2026: 40 · 2025: 47 · 2024: 65 · 2023: 71 · 2022: 88 · 2021: 94 · 2020: 94 · 2019: 136 · 2018: 107 · 2017: 67 · 2016: 13
- FWCI
- 29.23
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Nature Materials (publishedVersion)
- PubMed (publishedVersion)
- Rutgers University Community Repository (Rutgers University) (submittedVersion)
- HAL (submittedVersion)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › 2D Materials and Applications
- Physical Sciences › Engineering › Mechanical Engineering › Catalysis and Hydrodesulfurization Studies
- Keywords
- MoS2 nanosheets, hydrogen evolution reaction, electrocatalysis, 1T phase, charge injection, charge transport, sulfur vacancies, edge sites, phase engineering, monolayer transition metal dichalcogenides
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