The high spin-state and the three-coordinate Co geometry of 2 is quite unusual, as the vast majority of molecular Co III compounds are diamagnetic and five-or six-coordinate. Co[N(SiMe3)2]3 represents the only other example of a structurally characterized S = 2 Co III complex and its stability could be ascribed to the bulky amide ligands that occlude the coordination of additional ligands. The relatively large, positive value of D can be ascribed to the trigonal planar geometry in 2. Consistent with a large positive D, no EPR transitions were observed at X-band in both perpendicular and parallel mode; EPR transitions may be observable at much higher frequencies but such studies were not pursued. Electrochemical studies of 2 were pursued to understand the extent to which terminal PN ligation stabilizes the Co III oxidation state. The cyclic voltammogram (CV) of 2 in a THF electrolyte features an irreversible reduction at E = -1.67 V vs. Fc/Fc + , which can be assigned to the reduction to Co II (Fig ). An irreversible oxidation event at ~0 V is also observed and can be attributed to a Co III /Co IV redox couple or oxidation of the ligand framework. The electrochemical data of 2 can be compared to [Co III (TAML)] -, a Co III complex supported by a tetra-anionic, macrocyclic amide ligand. For [Co III (TAML)] -, the Co II /Co III couple was observed at -1.18 V vs. Fc/Fc + in a DCM electrolyte. The electrochemical data for 2 shows an enhanced stabilization (~0.5 V) of the Co III oxidation state as compared to anionic [Co III (TAML)] -. Accordingly, these data corroborate a hypothesis that terminally bound PN moieties quench the expected electrophilicity of Co III , and may explain the hesitancy of 2 to react with Lewis bases.