Hydrogen spillover in complex oxide multifunctional sites improves acidic hydrogen evolution electrocatalysis
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Abstract
Abstract Improving the catalytic efficiency of platinum (Pt) for hydrogen evolution reaction (HER) is crucial for water splitting technologies, and hydrogen spillover has emerged as a new frontier in designing the binary-component Pt/support HER electrocatalysts. However, such binary catalysts always suffer from long reaction pathway, undesirable interfacial barrier, and complicated synthesis processes. Here we report a single-phase complex oxide La2Sr2PtO7+δ as a high-performance HER electrocatalysts in acidic media via a unique atomic-scale hydrogen spillover effect between multifunctional catalytic sites. With insights from theoretical calculations, a possible synergistic mechanism involving the hydrogen spillover channel from OLa site→La-Pt bridge site→Pt site is proposed; namely, the OLa site enriches proton, the La-Pt bridge site with thermo-neutral H* adsorption facilitates the hydrogen spillover and H2 generation, and Pt site favors the final H2 desorption. Benefiting from such unusual phenomenon, the resulting La2Sr2PtO7+δ exhibits an exceptional HER electrode activity with low overpotential of 13 mV at 10 mA cm− 2 and small Tafel slope of 22 mV dec− 1, and significantly enhanced intrinsic activity and durability than commercial Pt black catalyst.
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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 [54]
The Results section (‘Experimental evidences for hydrogen spillover’; page unavailable) links a smaller hydrogen-desorption peak-shift slope to faster desorption and separately reports faster adsorption kinetics. Those findings concern La2Sr2PtO7+δ, not the HEA|Pt heterostructure; the cited passages also do not establish accelerated interfacial charge transfer for HEA|Pt. (LLM, conf=0.87)
Experimental — accuracy not yet measuredPlotting the hydrogen desorption peak position versus the scan rate is logical to quantify the hydrogen desorption kinetics.
“Therefore, plotting the hydrogen desorption peak position vs the scan rate was employed to compare the fitting slopes, which is logical to quantify the hydrogen desorption kinetics32.”
From Pd hydride metallene aerogels with lattice hydrogen participation for efficient hydrogen evolution reaction (2024) · cites this paper as [32]
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- Authors
- Dai, J., Zhu, Y., Chen, Y., Wen, X., Long, M., Wu, X., Hu, Z., Guan, D., Wang, X., Zhou, C., Lin, Q., Sun, Y., Weng, S.-C., Wang, H., Zhou, W., & Shao, Z.
- Affiliations
- Nanjing Tech University (CN)
- Monash University (AU)
- Shanghai Jiao Tong University (CN)
- Max Planck Institute for Chemical Physics of Solids (DE)
- Xiamen University (CN)
- National Synchrotron Radiation Research Center (TW)
- Corresponding author
- Zhu, Yinlong
- Shao, Zongping
- ORCID
- Venue
- Nature Communications
- Published
- 2022-03-04
- Volume
- 13
- Issue
- 1
- Pages
- 1189-1189
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC8897394
- OpenAlex
- W4214944543
- Cited by
- 467
- References
- 75
- Citations by year
- 2026: 90 · 2025: 144 · 2024: 131 · 2023: 73 · 2022: 29
- FWCI
- 16.98
- 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)
- Funders
- National Natural Science Foundation of China (21878158)
- 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 › Engineering › Electrical and Electronic Engineering › Fuel Cells and Related Materials
- Keywords
- hydrogen evolution reaction, hydrogen spillover, platinum-free electrocatalysts, acidic water splitting, proton adsorption, hydrogen migration, hydrogen desorption
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