Addition of the [NH] transfer reagent Hdbabh (dbabh = 2,3:5,6-dibenzo-7-azabicyclo[2.2.1]hepta-2,5-diene) to the bis(imino)pyridine iron bis(dinitrogen) complex, (((i)Pr)PDI)Fe(N(2))(2) (((i)Pr)PDI = 2,6-(2,6-(i)Pr(2)C(6)H(3)N horizontal lineCMe)(2)C(5)H(3)N), furnished the corresponding iron amide and ammonia compounds, resulting from cleavage of the strained amine. Isotopic labeling studies support N-H bond activation by a transient, parent imide, [(((i)Pr)PDI)FeNH].