We report the synthesis of α-diimine 1, 4-bis (2, 5-di-tert-butylphenyl)-2, 3-dimethyl-1, 4- diaza-1, 3-butadiene, 1, and α-iminoketones 2-[(3, 5-xylyl) imino] acenaphthylen-1-one, 4, and 2-[(4-chlorophenyl) imino] acenaphthylen-1-one, 5, all of which have been characterized by 1H NMR, 13C NMR, IR, and X-ray crystallography. Also, we report the previously unknown X-ray crystal structures of α-diimines Ar-BIAN (Ar-BIAN= bis ( ...