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Electronically Asynchronous Transition States for C–N Bond Formation by Electrophilic <b> [Co <sup>III</sup> (TAML)] </b> -Nitrene Radical Complexes Involving Substrate-to-Ligand Single-Electron Transfer and a Cobalt-Centered Spin Shuttle

Nicolaas P. van Leest, Martijn A. Tepaske, Bas Venderbosch, Jean‐Pierre H. Oudsen, Moniek Tromp, Jarl Ivar van der Vlugt, Bas de Bruin

2020ACS Catalysis47 citationsDOIOpen Access PDF

Abstract

= 1) cobalt(III) center. Hence, the TAML moiety can be regarded to act as a transient electron acceptor, the cobalt center behaves as a spin shuttle, and the nitrene radical acts as a nucleophile. Such a mechanism was hitherto unknown for cobalt-catalyzed hypovalent group transfer and the more general transition-metal-catalyzed nitrene transfer to alkenes but is now shown to complement the known concerted and stepwise mechanisms for N-group transfer.

Topics & Concepts

NitreneChemistryRadicalPhotochemistryLigand (biochemistry)Electron transferElectrophileRadical ionCatalysisMedicinal chemistryStereochemistryOrganic chemistryIonReceptorBiochemistrySynthesis and Catalytic ReactionsCatalytic C–H Functionalization MethodsMetal-Catalyzed Oxygenation Mechanisms