ArticleProceedings of the National Academy of Sciences of the United States of America2013
Experimental demonstration of radicaloid character in a Ru(V)=O intermediate in catalytic water oxidation.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 13 papers.
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13 citing papers in PubMed.
- Formation of a MnDalton transactions (Cambridge, England : 2003) · 2025Article
- Pentanuclear iron complex for water oxidation: spectroscopic analysis of reactive intermediates in solution and catalyst immobilization into the MOF-based photoanode.Journal of catalysis · 2024Article
- Ruthenium(v) terminal arylimido corroles: isolation, spectroscopic characterization and reactivity.Chemical science · 2023Article
- Computational Analysis of Structure - Activity Relationships in Highly Active Homogeneous Ruthenium-based Water Oxidation Catalysts.Catalysts (Basel, Switzerland) · 2022Article
- Promoting Proton Transfer and Stabilizing Intermediates in Catalytic Water Oxidation via Hydrophobic Outer Sphere Interactions.Chemistry (Weinheim an der Bergstrasse, Germany) · 2022Article
- Systematic Influence of Electronic Modification of Ligands on the Catalytic Rate of Water Oxidation by a Single-Site Ru-Based Catalyst.ChemSusChem · 2022Article
- XAS and EPR in Situ Observation of Ru(V) Oxo Intermediate in a Ru Water Oxidation Complex.ChemElectroChem · 2022Article
- Do multinuclear 3d metal catalysts achieve O-O bond formation via radical coupling or via water nucleophilic attack? WNA leads the way in [CoChem catalysis · 2021Article
- Atomically Dispersed Iridium on Indium Tin Oxide Efficiently Catalyzes Water Oxidation.ACS central science · 2020Article
- Article
- Isolation and Study of Ruthenium-Cobalt Oxo Cubanes Bearing a High-Valent, Terminal RuJournal of the American Chemical Society · 2019Article
- Unpaired electrons as probes of catalytic systems.Science progress · 2014Article
- Mechanism of Catalytic Water Oxidation by the Ruthenium Blue Dimer Catalyst: Comparative Study in D₂OMaterials (Basel, Switzerland) · 2013Article
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5 authors.
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Abstract
Water oxidation is the key half reaction in artificial photosynthesis. An absence of detailed mechanistic insight impedes design of new catalysts that are more reactive and more robust. A proposed paradigm leading to enhanced reactivity is the existence of oxyl radical intermediates capable of rapid water activation, but there is a dearth of experimental validation. Here, we show the radicaloid nature of an intermediate reactive toward formation of the O-O bond by assessing the spin density on the oxyl group by Electron Paramagnetic Resonance (EPR). In the study, an (17)O-labeled form of a highly oxidized, short-lived intermediate in the catalytic cycle of the water oxidation catalyst cis,cis-[(2,2-bipyridine)2(H2O)Ru(III)ORu(III)(OH2)(bpy)2](4+) was investigated. It contains Ru centers in oxidation states [4,5], has at least one Ru(V) = O unit, and shows
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