Hydrogen Spillover-Bridged Volmer/Tafel Processes Enabling Ampere-Level Current Density Alkaline Hydrogen Evolution Reaction under Low Overpotential
Open accessAbstract
Water-alkaline electrolysis holds a great promise for industry-scale hydrogen production but is hindered by the lack of enabling hydrogen evolution reaction electrocatalysts to operate at ampere-level current densities under low overpotentials. Here, we report the use of hydrogen spillover-bridged water dissociation/hydrogen formation processes occurring at the synergistically hybridized Ni 3 S 2 /Cr 2 S 3 sites to incapacitate the inhibition effect of high-current-density-induced high hydrogen coverage at the water dissociation site and concurrently promote Volmer/Tafel processes. The mechanistic insights critically important to enable ampere-level current density operation are depicted from the experimental and theoretical studies. The Volmer process is drastically boosted by the strong H 2 O adsorption at Cr 5c sites of Cr 2 S 3 , the efficient H 2 O* dissociation via a heterolytic cleavage process (Cr 5c -H 2 O* + S 3c (#) → Cr 5c -OH* + S 3c -H # ) on the Cr 5c /S 3c sites in Cr 2 S 3 , and the rapid desorption of OH* from Cr 5c sites of Cr 2 S 3 via a new water-assisted desorption mechanism (Cr 5c -OH* + H 2 O(aq) → Cr 5c -H 2 O* + OH - (aq)), while the efficient Tafel process is achieved through hydrogen spillover to rapidly transfer H # from the synergistically located H-rich site (Cr 2 S 3 ) to the H-deficient site (Ni 3 S 2 ) with excellent hydrogen formation activity. As a result, the hybridized Ni 3 S 2 /Cr 2 S 3 electrocatalyst can readily achieve a current densi…
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Adsorbed reaction intermediates in heterostructures can undergo spillover between adjacent components once a critical surface coverage is reached.
“adsorbed reaction intermediates in heterostructures can undergo spillover between adjacent components once a critical surface coverage is reached.16−18”
From High-Entropy Alloy Aerogels with High-Density Solid–Solid Heterointerfaces for Alkaline Hydrogen Evolution (2026) · cites this paper as [18]
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- Authors
- Fu, H. Q., Zhou, M., Liu, P. F., Liu, P., Yin, H., Sun, K. Z., Yang, H. G., Al-Mamun, M., Hu, P., Wang, H.-F., & Zhao, H.
- Affiliations
- Griffith University (AU)
- East China University of Science and Technology (CN)
- Centre for Catalysis and Clean Energy, Gold Coast Campus, Griffith University, Gold Coast, QLD 4222, Australia
- Queen's University Belfast (GB)
- Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China
- Corresponding author
- Yang, Hua Gui
- Zhao, Huijun
- ORCID
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2022-03-18
- Volume
- 144
- Issue
- 13
- Pages
- 6028-6039
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W4220862423
- Cited by
- 508
- References
- 5
- Citations by year
- 2026: 98 · 2025: 127 · 2024: 131 · 2023: 108 · 2022: 44
- FWCI
- 18.46
- Type
- journal article
- Language
- en
- Open access
- green
- hdl.handle.net
- Licence
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- Research Portal (Queen's University Belfast) (submittedVersion)
- Griffith Research Online (submittedVersion, other-oa)
- Funders
- Australian Research Council (DP200100965)
- National Natural Science Foundation of China (21873028, 51725201, 51920105003, 91945302, 92045303)
- Shanghai Shu Guang Project (17SG30)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Physical Sciences › Materials Science › Materials Chemistry › Hydrogen Storage and Materials
- Keywords
- hydrogen evolution reaction, alkaline water electrolysis, hydrogen spillover, water dissociation, heterolytic cleavage, OH desorption, hydrogen coverage, high current density, overpotential
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