Ammonia is an attractive medium for renewable hydrogen storage. Synthesis of ammonia via the Haber-Bosch process is already the second-largest chemical industrial process in the world, and as a result the infrastructure for ammonia storage and transport already exists. One significant bottleneck limiting the use of ammonia for hydrogen storage is the inability to efficiently extract hydrogen back from ammonia. Electrolysis offers a convenient route to decompose ammonia into nitrogen and hydrogen, which potentially only requires ca. 0.1 V. However, in practice, the overpotential of the ammonia oxidation (nitrogen evolution) half reaction is prohibitively large. We previously reported a transition metal complex, [Ru(tpy)(dmabpy)NH₃]²⁺ (tpy = 2,2′:6′,2′′-terpyridine, dmabpy = 4,4'-dimethylamino-2,2'-bipyridine), which exhibited electrocatalytic activity in presence of ammonia at room temperature and ambient pressure in an attempt to lower the overpotential. In this talk, recent efforts aimed at understanding the mechanism of the ammonia oxidation reaction using a variety of spectroscopic and electrochemical methods will be presented. Interestingly, reactions [Ru(tpy)(dmabpy)NH₃]³⁺ with various Lewis bases are shown to trigger a proposed redox disproportionation reaction, which was followed using variable temperature NMR. An intermediate species was identified as a dinitrogen bridged complex using ¹⁵N NMR and Raman spectroscopy on isotopically labeled complexes. This intermediate is proposed to derive from coupling of nitridyl species formed upon sequential redox disproportion reactions. Acetonitrile displaces the dinitrogen bridge to yield free N₂. DFT calculations support this lower energy pathway versus that previously reported for ammonia oxidation by the parent [Ru^III(tpy)(bpy)NH₃]³⁺ complex. These experimental and computational results are consistent with the interpretation of redox disproportionation involving sequential hydrogen atom transfer reactions by an amide/aminyl intermediate, [Ru(NH₂)]⁺, formed upon deprotonation of the parent complex. Analogous methylamine complexes, [Ru(NH₂CH₃)]^2+/3+, were also prepared to test the proposed mechanism. Treating [Ru(NH₂CH₃)]³⁺ with a Lewis base was found to cleanly yield two products [Ru(NH₂CH₃)]²⁺ and [Ru(CN)]⁺ in ~3:1 ratio, fully consistent with our proposed mechanism. In addition, preliminary results of next-generation catalyst systems will be presented.