A series of complexes with the general formula [M(6R-bpy)₃]²⁺ were prepared to explore the electronic properties (redox and spin state) as a function of varying (i) a substituent group on the 6-position on 2, 2'-bipyridine (6R-bpy) and (ii) the metal center [M represents Fe(II), Ru(II), and Os(II) metal centers]. The R-group on 2, 2'-bipyridne was varied as follows: R = H, CH3, Cl, and Br. The extent of influence of the R-substituent on the M(III/II) redox behavior was characterized by way of cyclic voltammetry using aprotic solvent conditions (acetonitrile) where each complex (except for Fe) was observed to have reversible behavior. The extent of influence of the R-group on the M(III/II) redox behavior was observed to be dependent on the metal center. NMR methodology was used for measuring room temperature magnetic susceptibilities of the Fe(II) complexes where considerable variation in spin behavior, both high (S = 2) and low (S = 0) spin states, was observed as a function of the R-group.