In the net sense, chemical and electrochemical oxidations of the ions [Ru(bpy)2(NFl2CH2R)2]2+ (NH2CH2R = allylamine, benzylamine, and zi-butylamine) occur by dehydrogenation at the amine ligands giving the corresponding bis(nitrile) complexes, [Ru(bpy)2(N=CR)2]2+. The reactions appear to proceed by initial oxidation of Ru(II) to Ru(III), followed by a series of stepwise dehydrogenation reactions which occur via imine intermediates.