Ionic liquids as new reaction media and catalysts have been experimentally and theoretically recognized and accepted.They are environmentally friendly or ‘‘greener’’ alternatives to organic solvents because they have very low vapor pressure and are non-explosive and thermally stable over a wide temperature range. They can be employed as solvents for a number of chemical processes, such as separation, reactions, two-phase catalysis, extractions6 and polymerizations. The application of ionic liquids as novel media may provide convenient solutions to both the solvent emission and catalyst reuse problem. One of the new applications of ionic liquids is in the synthesis of organic compounds including amides. Pyridinecarboxamide ligands have been part of the growing research in the filed of coordination chemistry of transition metal complexes. The solvent used in the (1) [Co(Me 2 )( prldn) 2 ] ClO 4 , (2) [Co(Me 2 )( bzlan) 2 ]ClO 4 , (3) [Co(Me 2 )( pprdn) 2 ]ClO 4 , (4) [Co(Me 2 )( mrpln) 2 ]ClO 4 , (5) [Co(Me 2 )( py) 2 ]PF 6 , (6) [Co(Me 2 )(3-MePy) 2 ] PF 6 , (7) [Co(Me 2 )( 3-AcPy) 2 ]ClO 4 (8) [Co(Me 2 )(N-MeIm) 2 ]ClO 4 have been synthesized and characteraized. Methyl groupes induce a higher ?-donating power to the equatorial ligand which in turn stimulates the bond formation between Co(III) and ?-acceptor amines. We have successfully to synthesized eight cobalt complexes with ?-acceptor axial ligands, that could not be synthesized with ligand. These complexes were characterized by UV-Vis, FT-IR, 1 HNMR and Elemental Analysis. Complexes 2 and 3 were structurally characterized by X-Ray Diffraction. The electrochemical properties of complexes 1-8 were also investigated by Cyclic Voltammetry, and the trend in the observed redox potentials was rationalized considering the axial ligand properties.