The complex [(FeO)-O-IV(N4Py)](2+) (N4Py = N,N-bis(2-pyridylmethyl)-N-bis(2- pyridyl)methylamine) has been prepared by bulk electrolysis in aqueous CH3CN and CH2Cl2, and its redox properties characterized. Bulk chronocoulometry and spectropotentiometry experiments in CH3CN show that [Fe-II(N4Py)(NCCH3)](2+) can be oxidized quantitatively to its iron(III) derivative at an applied potential of +0.71 V vs ferrocene and then to the oxoiron(IV) complex (in the presence of added water) at potentials above +1.3 V. The E-1/2 value for the Fe-IV/III couple has been estimated to be + 0.90 V from spectropotentiometric titrations in CH3CN and cyclic voltammetric measurements in CH2Cl2.