Construction of highly efficient and highly selective catalytic oxidation systems based on proton-coupled electron transfer

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We have established highly efficient and highly selective catalytic oxidation systems for organic substrates using Ru(II)-pyridylamine-aqua complexes as catalysts in aqueous buffer solutions. In those reactions, Ru(IV)-oxo complexes were formed via proton-coupled electron transfer and their characterization were made by spectroscopic and crystallographic methods and DFT calculations. In this research, we have clarified that the spin states of Ru(IV)-oxo complexes do not affect their reactivity. We have also succeeded in the direct observation of the oxygen-rebound mechanism in C-H hydroxylation for the first time and elucidated the reaction mechanism of C-H oxidation in the light of kinetic analysis.