Litcius/Paper detail

Proton-Coupled Electron-Transfer Reduction of Dioxygen: The Importance of Precursor Complex Formation between Electron Donor and Proton Donor

Yufan Wang, Ming‐Tian Zhang

2022Journal of the American Chemical Society40 citationsDOI

Abstract

The proton-coupled electron transfer (PCET) reaction has drawn extensive attention for its widespread occurrence in chemistry, biology, and materials science. The mechanistic studies via model systems such as tyrosine and phenol oxidation have gradually deepened the understanding of PCET reactions, which was widely accepted and applied to bond activation and transformation. However, direct PCET activation of nonpolar bonds such as the C–H bond, O2, and N2 has yet to be explored. Herein, we report that the interaction between electron donor and proton donor could overcome the barrier of direct O2 activation via a concerted electron–proton transfer mechanism. This work provides a new strategy for developing direct PCET activation of nonpolar bonds.

Topics & Concepts

ChemistryProton-coupled electron transferProtonElectron transferReduction (mathematics)ElectronPhotochemistryElectron donorCatalysisOrganic chemistryNuclear physicsGeometryMathematicsPhysicsMetal-Catalyzed Oxygenation MechanismsCO2 Reduction Techniques and CatalystsMetalloenzymes and iron-sulfur proteins