A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution
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Abstract
Hydrogen spillover phenomenon of metal-supported electrocatalysts can significantly impact their activity in hydrogen evolution reaction (HER). However, design of active electrocatalysts faces grand challenges due to the insufficient understandings on how to overcome this thermodynamically and kinetically adverse process. Here we theoretically profile that the interfacial charge accumulation induces by the large work function difference between metal and support (∆Φ) and sequentially strong interfacial proton adsorption construct a high energy barrier for hydrogen transfer. Theoretical simulations and control experiments rationalize that small ∆Φ induces interfacial charge dilution and relocation, thereby weakening interfacial proton adsorption and enabling efficient hydrogen spillover for HER. Experimentally, a series of Pt alloys-CoP catalysts with tailorable ∆Φ show a strong ∆Φ-dependent HER activity, in which PtIr/CoP with the smallest ∆Φ = 0.02 eV delivers the best HER performance. These findings have conclusively identified ∆Φ as the criterion in guiding the design of hydrogen spillover-based binary HER electrocatalysts.
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The reduced peak displacement indicates faster hydrogen adsorption and desorption kinetics on the HEA|Pt heterostructure, consistent with accelerated interfacial charge transfer processes.
“This reduced peak displacement indicates faster hydrogen adsorption and desorption kinetics on the HEA|Pt heterostructure, consistent with accelerated interfacial charge transfer processes.53−55”
From High-Entropy Alloy Aerogels with High-Density Solid–Solid Heterointerfaces for Alkaline Hydrogen Evolution (2026) · cites this paper as [55]
The Results section (‘Evidences for hydrogen spillover in Pt2Ir1/CoP’; page not provided) interprets a reduced hydrogen-desorption peak-shift slope as accelerated desorption kinetics. But it studies Pt2Ir1/CoP, not HEA|Pt, and does not establish that the peak displacement indicates faster adsorption kinetics or accelerated interfacial charge transfer in HEA|Pt. (LLM, conf=0.86)
Experimental — accuracy not yet measuredEIS-derived Tafel slopes under Ohm's law can estimate the hydrogen adsorption kinetics.
“Owing to the potential-dependent R2 for these electrocatalysts, plotting logR2 vs overpotential and corresponding the EIS-derived Tafel slopes under Ohm’s law can estimate the hydrogen adsorption kinetics30.”
From Pd hydride metallene aerogels with lattice hydrogen participation for efficient hydrogen evolution reaction (2024) · cites this paper as [30]
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- Authors
- Li, J., Hu, J., Zhang, M., Gou, W., Zhang, S., Chen, Z., Qu, Y., & Ma, Y.
- Affiliations
- Northwestern Polytechnical University (CN)
- Northwest University (CN)
- Xi'an Jiaotong University (CN)
- Nanyang Technological University (SG)
- Corresponding author
- Hu, Jun
- Qu, Yongquan
- Ma, Yuanyuan
- Venue
- Nature Communications
- Published
- 2021-06-09
- Volume
- 12
- Issue
- 1
- Pages
- 3502-3502
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC8190308
- OpenAlex
- W3137345457
- Cited by
- 633
- References
- 81
- Citations by year
- 2026: 114 · 2025: 192 · 2024: 169 · 2023: 109 · 2022: 43 · 2021: 6
- FWCI
- 15.33
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Locations
- Nature Communications (publishedVersion, cc-by)
- Research Square (acceptedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- DR-NTU (Nanyang Technological University) (submittedVersion)
- Funders
- China Postdoctoral Science Foundation (2018M640994)
- National Natural Science Foundation of China (21676216, Grants 21872109)
- 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 › Catalytic Processes in Materials Science
- Keywords
- hydrogen spillover, hydrogen evolution reaction, metal-support interface, work function difference, interfacial charge accumulation, electrocatalyst design, supported metal catalysts
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
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