A reinvestigation of the treatment of [Fe(N-2)(PP)(2)] (PP = depe, dmpe) with acid revealed no ammonium formation. Instead, rapid protonation at the metal center to give hydride Complexes was observed. Treatment of [Fe(N-2)(dmpe)(2)] with methylating agents such as methyl triflate or methyl tosylate resulted methylation of the metal center to afford [FeMe(N-2)(dmpe)(2)](+). Treatment of [Fe(N-2)(dmpe)(2)] With trimethylsilyl triflate, however, resulted in reactibn at dinitrogen affording NH4+ on subsequent treatment with acid. The side-on bound hydrazine complex [Fe-(N2H4)(dmpe)(2)](2+) and bis(ammonia) complex [Fe(NH3)(2)(dmpe)(2)](2+) were identified by N-15 NMR spectroscopy as other species formed in the reaction mixture.