Iron‐Catalyzed Reductive Alkylation of Imines via Ligand‐to‐Metal Charge Transfer

Abstract Herein, we report a sustainable, iron‐catalyzed reductive alkylation reaction of imines with carboxylic acids and unactivated hydrocarbons to access synthetically relevant amine motifs. The reaction proceeds via a light‐induced ligand‐to‐metal charge transfer (LMCT) process, generating alkyl radicals either through a decarboxylative pathway or by forming a reactive chlorine radical that facilitates hydrogen atom transfer (HAT) with alkanes. This photochemical transformation offers several advantages, including sustainability, mild reaction conditions, cost efficiency, and an excellent atom economy.