Inverse kinetic isotope effects in the oxygen reduction reaction at platinum single crystals
Open accessAbstract
Although the oxygen reduction reaction (ORR) involves multiple proton-coupled electron transfer processes, early studies reported the absence of kinetic isotope effects (KIEs) on polycrystalline platinum, probably due to the use of unpurified D 2 O. Here we developed a methodology to prepare ultra-pure D 2 O, which is indispensable for reliably investigating extremely surface-sensitive platinum single crystals. We find that Pt(111) exhibits much higher ORR activity in D 2 O than in H 2 O, with potential-dependent inverse KIEs of ~0.5, whereas Pt(100) and Pt(110) exhibit potential-independent inverse KIEs of ~0.8. Such inverse KIEs are closely correlated to the lower *OD coverage and weakened *OD binding strength relative to *OH, which, based on theoretical calculations, are attributed to the differences in their zero-point energies. This study suggests that the competing adsorption between *OH/*OD and *O 2 probably plays an important role in the ORR rate-determining steps that involve a chemical step preceding an electrochemical step (CE mechanism).
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Inverse KIE behavior reported for oxygen reduction on Pt single crystals is attributed to weaker *OD binding and reduced *OD surface coverage relative to *OH, arising from competitive adsorption effects.
“Similar inverse KIE behavior has been reported for oxygen reduction on Pt single crystals and has been attributed to weaker *OD binding and reduced *OD surface coverage relative to *OH, arising from competitive adsorption effects.56”
From High-Entropy Alloy Aerogels with High-Density Solid–Solid Heterointerfaces for Alkaline Hydrogen Evolution (2026) · cites this paper as [56]
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“…density of the KOH + H 2 O and KOD + D 2 O electrolyte systems, PdH 0.45 Cu/CNT and PdH 0.68 /CNT are calculated to exhibit the high KIE value, accelerating proton transfer and enabling the electrophilic *HCOO to nucleophilic *C(OH) 2 conversion process with excellent kinetic performance [56 ].”
InfluentialDistinguishing concerted and sequential proton-electron transfer.
Carlson, E., & Chueh, W. C. (2026) · Nature Chemistry · doi:10.1038/s41557-026-02103-y
Guo, W.-B., Yang, R., Fan, J.-Y., Xiang, X., Du, X.-M., Shi, N.-E., Bao, J., & Han, M. (2024) · RSC Advances · doi:10.1039/d3ra07657a
Zhang, J.-J., Wang, J., Fu, Y.-M., Cao, L.-S., Peng, X., Huang, G.-J., Peng, W.-D., Wu, C., Liang, Y.-W., Wei, W.-G., et al. (2026) · Journal of Materials Chemistry A · doi:10.1039/d6ta00692b
WO3-induced K+-enriched electrical double layer for accelerated alkaline hydrogen evolution
Kim, K., Jung, K., Yoon, H., Park, Y., Haryanto, A., An, S., Sung, K.-C., Lee, C.-W., & Kim, D.-W. (2026) · Applied Catalysis B: Environment and Energy · doi:10.1016/j.apcatb.2026.127477
- Authors
- Yang, Y., Agarwal, R. G., Hutchison, P., Rizo, R., Soudackov, A. V., Lu, X., Herrero, E., Feliu, J. M., Hammes-Schiffer, S., Mayer, J. M., & Abruña, H. D.
- Affiliations
- Cornell University (US)
- Yale University (US)
- University of Alicante (ES)
- ORCID
- Venue
- Nature Chemistry
- Published
- 2022-11-10
- Volume
- 15
- Issue
- 2
- Pages
- 271-277
- ISSN
- 1755-4330 (ISSN-L)
- 1755-4349
- OpenAlex
- W4308772436
- Cited by
- 123
- References
- 0
- Citations by year
- 2026: 27 · 2025: 40 · 2024: 39 · 2023: 17
- FWCI
- 4.33
- Type
- journal article
- Language
- en
- Open access
- green
- hdl.handle.net
- Licence
- Locations
- Nature Chemistry (publishedVersion)
- PubMed (publishedVersion)
- RUA, Repositorio Institucional de la Universidad de Alicante (Universidad de Alicante) (submittedVersion)
- Funders
- U.S. Department of Defense (FA95501810497, FA95501810420)
- U.S. Department of Energy (DESC0019445)
- Ministerio de Ciencia e Innovación
- Multidisciplinary University Research Initiative (FA9550-18-1-0420)
- 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
- inverse kinetic isotope effect, oxygen reduction reaction, platinum single crystals, reaction mechanism, electrocatalysis, hydrogen evolution reaction
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