Publication date: 15th December 2025
Synthesis of green NH3 enables the possibility of producing carbon-free, high energy density liquid fuel on the TW scale. The HB reaction is almost thermoneutral, which means hydrogen’s intrinsic energy is largely retained in ammonia, making NH3 an ideal candidate for storing and transporting renewable H2. The conversion of NH3 to electricity via a direct ammonia fuel cell or back to H2 via electrolysis has received little attention until very recently, however, and is primarily limited by the ammonia oxidation reaction (AOR). This talk will present results from our investigations into homogeneous electrocatalysts to drive the AOR at room temperature and ambient pressure. Our group reported the first example of a homogenous electrocatalyst for ammonia oxidation under mild conditions; [Ru(tpy)(dmabpy)NH3]2+ (tpy = terpyridine; dmabpy = 4,4′-bis(dimethylamino)-2,2′-bipyridine), [Ru(NH3)]2+. Electrocatalytic behavior of [Ru(NH3)]2+ will be presented with complementary spectroscopic (NMR and optical) methods of stoichiometric reactions using isotope labeling to unravel the mechanism(s) of AOR. Recent results of the surprising catalytic behavior of the coordinatively saturated [Ru(Cl)]+ complex will also be presented. The reaction of [Ru(Cl)]2+ with NH3 is surprisingly clean and does not form any [Ru(NH3)]2+ as a side product when carried out in MeCN-d3. 1H and 15N NMR spectroscopy measurements show the products of the reaction are only [Ru(Cl)]+ and N2. Preliminary results of other coordinatively saturated complexes will also be introduced with similar behavior. Taken together, these recent results suggest a third operative pathway of AOR triggered by a one-electron oxidation reaction. In addition, recent efforts to determine the overpotential of the AOR reaction using OCP measurements in a series of non-aqueous solvents titrated with NH₄⁺/NH₃ will be presented. An alternative approach will then be introduced, using differential potentiometric measurements to determine the universal 
values aligned to the aqueous pH scale for dilute NH₄⁺/NH₃ solutions in the same solvents: MeCN, THF, DMF, and PC. Knowledge of the values allows simple determination of the reversible hydrogen potential in any given solvent relative to the aqueous standard hydrogen electrode, SHE. The close agreement of these two methods, as well as calculated potentials from literature values when available, substantiates the new, simpler and more robust approach to determine the reversible hydrogen potential introduced here. We further use the reversible hydrogen potential values established here to report the overpotential for ammonia oxidation as a function of solvent with the ruthenium-based molecular catalysts described above.
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