A novel catalytic system including NiCl2‐NHC ligand precursor has been developed for the preparation of imines from amines and ketones from alcohols. Owing to the acceptorless dehydrogenation pathway for this reaction, the hydrogen gas is liberated as a by‐product. The active catalyst is generated in situ by the reaction of nickel (II) chloride, bis (imidazolium) chlorides and potassium tert‐butoxide. The products were obtained in good to excellent yields and a wide variety of amines and ketones were applied successfully in this protocol.
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