Iridium-catalyzed electrochemical C-H activation was accomplished within a cooperative catalysis manifold, setting the stage for electrooxidative C-H alkenylations through weak O-coordination. The iridium-electrocatalyzed C-H activation featured high functional-group tolerance through assistance of a metal-free redox mediator through indirect electrolysis. Detailed mechanistic insights provided strong support for an organometallic C-H cleavage and a synergistic iridium(III/I)/redox catalyst regime, enabling the use of sustainable electricity as the terminal oxidant with improved selectivity features.
Keywords: C−H activation; Redox catalysts; electrochemistry; iridium catalysis; selectivity.
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