ArticleNature chemistry2024
Operando film-electrochemical EPR spectroscopy tracks radical intermediates in surface-immobilized catalysts.
Article in Nature chemistry, 2024. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 15 papers.
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Who cites it
15 citing papers in PubMed.
- EPR spectroscopy 80 years after its discovery.Science advances · 2026Review
- F-centre charge state and dynamism govern oxide electrocatalytic selectivity.Nature chemistry · 2026Article
- CEEN: A Control Software for Coupled Electrochemistry, EPR, and NMR for Redox Flow Battery and Electrosynthesis Research.Magnetic resonance in chemistry : MRC · 2026Article
- Amide-engineered copper nitride for shortcut-pathway-locked electroreduction of concentrated hydroxymethylfurfural.Nature communications · 2026Article
- Electron hopping in conjugated molecular wires with application to solar cells.Nature chemistry · 2026Article
- Versatile High-Sensitivity EPR Using Superconducting Spiral Microresonators.Small methods · 2026Article
- Lessons, connections, hypotheses and predictions from protein film electrochemistry.Journal of biological inorganic chemistry : JBIC : a publication of the Society of Biological Inorganic Chemistry · 2026Review
- Radical Electroprecipitation from a Water|Oil|Electrode Interface Prolongs "Electro"Chemiluminescence of the Tris(2,2'-bipyridyl)Ruthenium(II) and Benzoyl Peroxide System by 10Angewandte Chemie (International ed. in English) · 2026Article
- Sequential-chain coupling over hierarchical click-sites enables highly selective urea electrosynthesis.Nature communications · 2026Article
- Enhanced Resolution in EPR Spectroscopy Using para-Hydrogen Matrices.Angewandte Chemie (International ed. in English) · 2026Article
- Isotopic and defect analysis of enriched molybdenum oxide using EPR spectroscopy and DFT simulation.Scientific reports · 2026Article
- Decoupling of Spin and Non-Spin Effects From Electronic Structure Modulation for Oxygen Electrocatalysis.Advanced science (Weinheim, Baden-Wurttemberg, Germany) · 2025Review
- Single Atom Engineering for Electrocatalysis: Fundamentals and Applications.ACS catalysis · 2025Review
- Design of an Electrochemical Cell for Continuous Wave EPR Measurements of Radical Ions.Chemistry (Weinheim an der Bergstrasse, Germany) · 2024Article
- Noble Metal Plasmon-Molecular Catalyst Hybrids for Renewable Energy Relevant Small Molecule Activation.ACS nanoscience Au · 2024Review
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Authors and funding
7 authors.
Funding
Abstract
The development of surface-immobilized molecular redox catalysts is an emerging research field with promising applications in sustainable chemistry. In electrocatalysis, paramagnetic species are often key intermediates in the mechanistic cycle but are inherently difficult to detect and follow by conventional in situ techniques. We report a new method, operando film-electrochemical electron paramagnetic resonance spectroscopy (FE-EPR), which enables mechanistic studies of surface-immobilized electrocatalysts. This technique enables radicals formed during redox reactions to be followed in real time under flow conditions, at room temperature and in aqueous solution. Detailed insight into surface-immobilized catalysts, as exemplified here through alcohol oxidation catalysis by a surface-immobilized nitroxide, is possible by detecting active-site paramagnetic species sensitively and quantitatively operando, thereby enabling resolution of the reaction kinetics. Our finding that the surface electron-transfer rate, which is of the same order of magnitude as the rate of catalysis (accessible from operando FE-EPR), limits catalytic efficiency has implications for the future design of better surface-immobilized catalysts.
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