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Electrooxidative Rhodium‐Catalyzed [5+2] Annulations via C−H/O−H Activations

Yulei Wang, João C. A. Oliveira, Zhipeng Lin, Lutz Ackermann

2021Angewandte Chemie International Edition90 citationsDOIOpen Access PDF

Abstract

Electrooxidative annulations involving mild transition metal-catalyzed C-H activation have emerged as a transformative strategy for the rapid construction of five- and six-membered heterocycles. In contrast, we herein describe the first electrochemical metal-catalyzed [5+2] cycloadditions to assemble valuable seven-membered benzoxepine skeletons by C-H/O-H activation. The efficient alkyne annulation featured ample substrate scope, using electricity as the only oxidant. Mechanistic studies provided strong support for a rhodium(III/I) regime, involving a benzoxepine-coordinated rhodium(I) sandwich complex as the catalyst resting state, which was re-oxidized to rhodium(III) by anodic oxidation.

Topics & Concepts

RhodiumCatalysisChemistryMedicinal chemistryOrganic chemistryCatalytic C–H Functionalization MethodsRadical Photochemical ReactionsSynthesis and Catalytic Reactions
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