Coordination-number dependence of reactivity in an imidoiron(III) complex

(Chemical Equation Presented) Reaction of the {LMeFe} fragment with adamantyl azide (AdN3) in the presence of 4-tert-butylpyridine (tBuPy) gives an S = 3/2 species that has been examined by 1H NMR, IR, EPR, and Mössbauer spectroscopies. DFT calculations point toward an identification as [LMeFeNAd]. This species abstracts hydrogen atoms from the ligand or external reagents only through its pyridine adduct (see scheme; Ar = 2,6-iPr2C6H3). © 2006 Wiley-VCH Verlag GmbH & Co. KGaA.