Angewandte Chemie International Edition · 2019 · 146 citations · 37 references
Natural SciencesChemistryMedicinal ChemistryBiocatalysisCatalysisSynthetic Medicinal ChemistryCatalyst DesignCatalytic MechanismsPhotocatalysisPhotochemistryRadical ReactionsReaction MechanismsCatalytic Reaction MechanismsPhotocatalytic SynthesisPhotoredox CatalysisPhotoredox Cross-couplingPhotoredox FunctionalizationRadical Mediated C - H FunctionalizationSide Reactions
The synthetic utility of tertiary amines to oxidatively generate α-amino radicals is well established, however, primary amines remain challenging because of competitive side reactions. This report describes the site-selective α-functionalization of primary amine derivatives through the generation of α-amino radical intermediates. Employing visible-light photoredox catalysis, primary sulfonamides are coupled with electron-deficient alkenes to efficiently and mildly construct C-C bonds. Interestingly, a divergence between intermolecular hydrogen-atom transfer (HAT) catalysis and intramolecular [1,5] HAT was observed through precise manipulation of the protecting group. This dichotomy was leveraged to achieve excellent α/δ site-selectivity.
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Catalytic alkylation of remote C–H bonds enabled by proton-coupled electron transfer
Gilbert J. Choi, Qilei Zhu, David C. Miller et al. · Nature · 2016 · 770 citations · Full text