Coordination‐Number Dependence of Reactivity in an Imidoiron(III) Complex

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).