Dedicated to Professor Peter W. Roesky on the occasion of his 55 th Birthday.Three zinc complexes, with the general formula {ksupported by a neutral iminopyrrole-morpholine ligand, were synthesized by the reaction between 1) and anhydrous zinc dihalides (ZnCl 2 , ZnBr 2 , ZnI 2 ) at ambient temperature in dry methanol. The zinc complexes were fully characterized using multinuclear NMR spectroscopic techniques and the molecular structures of complexes 2 a and 2 c in their solid states were determined by single-crystal X-ray diffraction analysis. The zinc diiodo complex (2 c) proved to be a competent precatalyst in the formation of a wide range of benzimidazole and benzothiazole compounds, via aerobic oxidative condensation of several benzylamines with o-phenylenediamine, N-phenyl-o-phenylene-diamine, and o-mercaptoaniline. The benzimidazole and benzothiazole derivatives were successfully characterized using 1 H and 13 C{ 1 H} NMR spectroscopy.

Two bench stable palladium(II) complexes [k2-(PyCH=N(CHPh2)PdCl2)] (1) and [k3-(PyCH=N(CH(Ph2)(C6H4))PdCl)] (2) supported by iminopyridine ligands (PyCH=NR) [R = CHPh2, (L1) and R = CPh3, (L2)] were synthesized and utilized as the competent catalysts in the formation of C-C coupling products for Suzuki-Miyaura and Heck-Mizoroki reactions. The palladium complex 1 was obtained by the k2 coordination of the ligand L1 to the palladium precursor whereas complex 2 was achieved by ortho-metallation of one of the phenyl groups present in ligand L2 with the Pd metal under reaction conditions making the ligand k3-ligation to the metal. Complex 2 exhibited excellent catalytic efficiency at very low catalyst loading (0.5 mol%). The new C-C bond formations of the desired products were obtained in high yield at mild reaction conditions. Wide varieties of substrate scopes were explored for the C-C bond cross-coupling reactions.