Manipulating Coordination Structures of Mixed-Valence Copper Single Atoms on 1T-MoS2 for Efficient Hydrogen Evolution
Abstract
Directing single atoms (SAs) to occupy specific lattice sites in support materials and correlating the resulting changes in atomic coordination structures to catalytic activity are crucial for the rational design of high-performance single-atom catalysts (SACs). Herein, for the same copper (Cu) SAs, two coordination structures on 1T-phase molybdenum disulfide (MoS 2 ) are identified. In the adsorption model, Cu SAs are coordinated onto the outermost sulfur (S) plane in a trigonal pyramidal geometry (Cu ads @MoS 2 ), while in the substitution model, Cu SAs are substituted with molybdenum (Mo) atoms (Cu sub @MoS 2 ), octahedrally coordinating with six S atoms in 1T-MoS 2 . Interestingly, in both coordination models, Cu(I) and Cu(II) SAs simultaneously exist. Cu ads @MoS 2 (173 mV) and Cu sub @MoS 2 (160 mV) demonstrate significantly reduced overpotential (at 10 mA cm –2 ) for the hydrogen evolution reaction (HER) compared to that of 1T-MoS 2 (235 mV) under acidic condition (0.5 M H 2 SO 4 ). Additionally, theoretical results reveal that different coordination structures would result in distinct active sites, where in Cu ads @MoS 2, the Cu SAs are the active sites, whereas in Cu sub @MoS 2, the S atoms most adjacent to the Cu SAs are the major active sites. Accurately determining the atomic coordination structures of SAs and uncovering their structure–property relationships are essential to guiding future geometry and structural research on SACs.
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The electrocatalytic performance of MoS2/Etched-SiCNWA is competitive with electrocatalysts reported recently.
“the electrocatalytic performance of MoS2/Etched-SiCNWA is competitive with the electrocatalyst reported recently [53–57] (Table S1)”
From Defect-induced growth of MoS2 nanosheets on selectively etched SiC nanowires aerogel for efficient electrocatalytic hydrogen evolution (2025) · cites this paper as [54]
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Self-citation
- Authors
- Li, Z., Yan, X., He, D., Hu, W., Younan, S., Ke, Z., Patrick, M., Xiao, X., Huang, J., Wu, H., Pan, X., & Gu, J.
- Affiliations
- San Diego State University (US)
- University of California, Irvine (US)
- Wuhan University (CN)
- Marquette University (US)
- Corresponding author
- Wu, Hongjun
- Pan, Xiaoqing
- Gu, Jing
- ORCID
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2022-06-14
- Volume
- 12
- Issue
- 13
- Pages
- 7687-7695
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W4282826880
- Cited by
- 83
- References
- 52
- Citations by year
- 2026: 19 · 2025: 23 · 2024: 18 · 2023: 19 · 2022: 4
- FWCI
- 2.88
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- ACS Catalysis (publishedVersion)
- Funders
- Division of Chemistry (CHE- 1955786)
- Natural Science Foundation of Heilongjiang Province (JC2017002)
- San Diego State University
- Northeast Petroleum University (GLJHB201901)
- Division of Chemical, Bioengineering, Environmental, and Transport Systems (CBET 1704992, CBET-2031494)
- National Natural Science Foundation of China (21476046)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Keywords
- copper single-atom catalysts, 1T-MoS2, hydrogen evolution reaction, coordination structure, mixed-valence copper, trigonal pyramidal coordination, octahedral coordination, sulfur adsorption, molybdenum substitution, active site, structure-activity relationship, acidic electrocatalysis
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