Unnatural Amino Acid Synthesis Enabled by the Regioselective Cobalt(III)‐Catalyzed Intermolecular Carboamination of Alkenes

Abstract Herein, we report an unprecedented regioselective and entirely atom‐economic cobalt(III)‐catalyzed method for the non‐annulative, intermolecular carboamination of alkenes. The methodology enables the direct synthesis of unnatural amino acid derivatives and proceeds under redox‐neutral conditions with a completely regioselective C−C bond and C−N bond formation. Furthermore, this reaction exemplifies the inherently different mechanistic behavior of the Cp*Co III catalyst and its Cp*Rh III counterpart, especially towards β‐H‐elimination.