ArticleNature chemistry2025
High-pressure pump-probe experiments reveal the mechanism of excited-state proton-coupled electron transfer and a shift from stepwise to concerted pathways.
Article in Nature chemistry, 2025. The graph could read no effect estimate from its abstract, so it casts no vote on the map. An erratum has been issued. Cited by 5 papers.
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Who cites it
5 citing papers in PubMed.
- Electronic and solvent reorganization in proton-coupled electron transfer captured by ultrafast X-rays.Nature communications · 2026Article
- Directional Concerted Proton-Electron Transfer in COFs for Efficient Photocatalytic HAdvanced materials (Deerfield Beach, Fla.) · 2026Article
- Activation volumes associated with excited-state electron transfer across amidinium-carboxylate bridge.Chemical science · 2026Article
- Unveiling a proton-coupled electron-transfer mechanistic library of nitrate to ammonia via ultramicroelectrode-hyphenated mass spectrometry.Proceedings of the National Academy of Sciences of the United States of America · 2026Article
- High-pressure pump-probe experiments reveal the mechanism of excited-state proton-coupled electron transfer and a shift from stepwise to concerted pathways.Nature chemistry · 2025Article
Corrections and comments
- Erratum issued
Authors and funding
7 authors.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Chemical energy conversion and storage in natural and artificial systems rely on proton-coupled electron transfer (PCET) processes. Concerted proton-electron transfer (CPET) can provide kinetic advantages over stepwise processes (electron transfer (ET)/proton transfer (PT) or PT/ET), so understanding how to distinguish and modulate these processes is important for their associated applications. Here, we examined PCET from the excited state of a ruthenium complex under high pressures. At lower buffer or quencher concentrations, a stepwise PT/ET mechanism was observed. With increasing pressure, PT slowed and ET sped up, indicating a merging of the two steps. In contrast, CPET at higher concentrations of buffer or quencher showed no pressure dependence of the reaction rate. This is because the simultaneous transfer of electrons and protons circumvents changes in charges and, consequently, in solvent electrostriction during the transition state. Our findings demonstrate that pressure can serve as a tool to monitor charge changes along PCET pathways, aiding in the identification of its mechanisms.
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Registered trials
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