Palladium on Carbon Nitride as a Recyclable Catalyst for Base‐Free N‐Benzylation of Anilines

A heterogeneous palladium‐catalyzed N‐benzylation of anilines is introduced, utilizing alcohols via borrowing hydrogen methodology under base and ligand‐free conditions. The spectroscopic and analytical characterization of the catalyst demonstrated the presence of Pd nanoparticle grafted on the carbon nitride with 2–5 nm size. A wide range of functional groups is tolerated under the current protocol. Additionally, the catalyst could be employed to synthesize 2‐phenyl benzimidazole using o ‐phenyl diamine and alcohol via dehydrogenative cyclization. Furthermore, the large‐scale utility of the catalyst on gram‐scale synthesis has been performed along with several controlled experiments to delineate the underlying mechanism.