Linear Selective C-H Bond Alkylation with Activated Olefins Catalyzed by Cp*CoIII

A simple and efficient method for Cp*Co-III-catalyzed C-H bond alkylation using activated olefins was developed. Selective C-H monoalkylation was performed at ambient temperature. One-pot symmetrical dialkylation and sequential unsymmetrical C-H dialkylation were performed to give the desired products in excellent yields. The reaction was found to proceed through an M-alkyl intermediate after migratory insertion, and this intermediate undergoes protodemetalation to give the expected alkylated product along with the regenerated catalyst.