Treatment of A in C6D6 with a stoichiometric amount of pyridine at ambient temperature led to full conversation into a new paramagnetic species within 5 minutes as observed by 1 H NMR spectroscopy. The solution phase magnetic susceptibility measurement (Evan's method) of this species (C6D6, 25 °C) of 2.68 µB is consistent with an S = 1 ground state. distorted trigonal bipyramidal geometry (t 5 = 0.87, Figure ). The solid-state structure identified coordination through the nitrogen of the pyridine to the iron center, while the aromaticity of the pyridine ring is maintained. Analysis of bond metrics shows the Fe-N bond distance (2.0600(16) Å) is comparable to that found for the related system reported by Wang (2.040(3) Å). 26 The addition of benzonitrile (1 equiv.) to complex A in C6D6 resulted in a rapid color change from dark red to black at ambient temperature. The resulting mononuclear complex [{( iPr DPB Ph )Fe(NCPh)}], 7, was characterized by X-ray crystallographic analysis. Benzonitrile coordinates to the iron center through the nitrogen atom, retaining the triple bond character of the C-N bond (1.154(3) Å) as also evidenced by ATR-FTIR which shows an absorbance centered at 2149 cm -1 . In this highly distorted trigonal bipyramidal (t 5 = 0.67) complex, the Fe-N-C32 bond deviates slightly from linearity 166.88(19)°, which is consistent with other examples found in the literature. The solution magnetic moment (C6D6, 25 °C) of 2.54 µB was found to be lower than expected for a typical S = 1 species. A stoichiometric reaction of 7 with HBpin at ambient temperature afforded 3d exclusively within 6 hours. The iron(0) species then binds dinitrogen and is converted back to complex A, as observed by 1 H NMR spectroscopy. To elucidate if complex 7 was part of the catalytic cycle, complex A was substituted for 7 under the same catalytic conditions for nitrile hydroboration and gave comparable yields and performance. Preliminary kinetic studies using initial rates were carried out using benzonitrile and complex A, following the growth of the hydroboration product, 3d by 1 H NMR spectroscopy at 50 °C. We observed a half-order dependency for complex A, attributed to the dissociation of A into monomeric form.