Nickel‐Catalyzed Electrooxidative C−H Amination: Support for Nickel(IV)

Nickel‐catalyzed electrochemical C−H aminations were accomplished by chemo‐ and position‐selective C−H activation with ample scope. Detailed mechanistic studies highlighted a facile C−H cleavage with unique chemo‐selectivity, while cyclovoltammetric analysis provided support for a nickel(II/III/IV) manifold. II…III…IV: Nickel‐catalyzed C−H aminations proved viable with electricity as the sole oxidant by fast C−H cleavage involving nickel(IV) species.