Engineering the Composition and Crystallinity of Molybdenum Sulfide for High-Performance Electrocatalytic Hydrogen Evolution
Abstract
The key challenge for the development of high-performance molybdenum sulfide HER catalysts lies in the limited fundamental understanding for the correlation between the catalytic activities and physical features of the materials. Here we have demonstrated an unambiguous correlation between the catalytic performance and the composition/crystallinity of molybdenum sulfide. The results indicate that the crystallinity plays an overwhelming role in determining the catalytic performance, while the composition does not matter much. The crystallinity can affect the three figures of merit of the catalytic performance (Tafel slope, turnover frequency (TOF), and stability) in opposite directions. Generally, the materials with low crystalline quality may provide low Tafel slopes (∼40 mV/dec), while highly crystalline molybdenum sulfide shows higher TOFs (by 2 orders of magnitude) and better stability. DFT calculations suggest that the terminal disulfur complex S 2 2–, which may exist in MoS 3 and also likely MoS 2 of low crystalline quality due to its structural disorder, could be the true catalytically active site responsible for the low Tafel slope. Our results indicate that one key issue for the rational design of high-performance molybdenum sulfide HER catalysts is to engineer the crystallinity such that balancing its contradictory effects on the different aspects of the catalytic performance. We show that nanocrystalline MoS 2 with few-layer nanoclusters in a lateral size of 5–30 nm…
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MoS2 has received tremendous attention owing to its high activity and earth-abundant composition.
“Among all these TMDs, molybdenum disulfide (MoS2) has received tremendous attention owing to the high activity and earth-abundant composition, inducing the rapid development of various kinds of MoS2-based HER electrocatalysts [19–23].”
From Graphene/graphene nanoribbon aerogels as tunable three-dimensional framework for efficient hydrogen evolution reaction (2017) · cites this paper as [23]
MoS2 can be a promising electrocatalyst for HER.
“Recently, researchers have found that MoS2 can be a promising electrocatalyst for HER.22−31”
From In-Situ Growth of Few-Layered MoS<sub>2</sub> Nanosheets on Highly Porous Carbon Aerogel as Advanced Electrocatalysts for Hydrogen Evolution Reaction (2015) · cites this paper as [27]
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All The Catalytic Active Sites of MoS <sub>2</sub> for Hydrogen Evolution
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- Authors
- Li, Y., Yu, Y., Huang, Y., Nielsen, R. A., Goddard, W. A., Li, Y., & Cao, L.
- Affiliations
- North Carolina State University (US)
- California Institute of Technology (US)
- Corresponding author
- Li, Yanpeng
- Cao, Linyou
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-12-17
- Volume
- 5
- Issue
- 1
- Pages
- 448-455
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W1983776877
- Cited by
- 155
- References
- 7
- Citations by year
- 2026: 2 · 2025: 3 · 2024: 10 · 2023: 7 · 2022: 10 · 2021: 13 · 2020: 20 · 2019: 12 · 2018: 21 · 2017: 22 · 2016: 23 · 2015: 12
- FWCI
- 6.27
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- ACS Catalysis (publishedVersion)
- CaltechAUTHORS (California Institute of Technology) (submittedVersion)
- Funders
- Basic Energy Sciences (DE-SC0012575)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Engineering › Mechanical Engineering › Catalysis and Hydrodesulfurization Studies
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Metalloenzymes and iron-sulfur proteins
- Keywords
- molybdenum sulfide, hydrogen evolution reaction, electrocatalysis, crystallinity, Tafel slope, turnover frequency, catalyst stability, amorphous MoS2, molybdenum trisulfide, composition effects, rational catalyst design
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