Treatment of the bis(imino)pyridine molybdenum eta(6)-benzene complex ((PDI)-P-iPr)Mo(eta(6)-C6H6) ((PDI)-P-iPr, 2,6-(2,6-iPr(2)C(6)H(3)N-CMe)(2)C5H3N) with NH3 resulted in coordination induced haptotropic rearrangement of the arene to form ((PDI)-P-iPr)Mo(NH3)(2)(eta(2)-C(6)H6()). Analogous eta(2)-ethylene and eta(2)-cyclohexene complexes were also synthesized, and the latter was crystallographically characterized. All three compounds undergo loss of the eta(2)-coordinated ligand followed by N-H bond activation, bis(imino)pyridine modification, and H-2 loss. A dual ammonia activation approach has been discovered whereby reversible M-L cooperativity and coordination induced bond weakening likely contribute to dihydrogen formation. Significantly, the weakened N-H bonds in ((PDI)-P-iPr)Mo(NH3)2(eta(2)-C2H4) enabled hydrogen atom abstraction and synthesis of a terminal nitride from coordinated ammonia, a key step in NH3 oxidation.