A series of tridentate diaryl imine ligands are appended to iron via C-H bond activation utilizing (Me3P)4FeMe2. The compounds generated selectively bind N2 from the air, with dinitrogen replacing a PMe3 ligand. The general chemistry of these species, including the preparation of related Fe(III) complexes, will be discussed. An alternative strategy toward C-C bond formation involves the generation of transient radicals that can couple at or around one or more metal centers.