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Transition metal nitrides have shown promise as electrocatalysts in proton exchange membrane fuel cells and electrolyzers, but the instability of these nitrides in acid has limited their function for such technologies. On the other hand, having fast, complete nitride dissolution and ammonia formation in acid can offer new opportunities for distributed, on-demand ammonia generation. Optimizing nitride chemistries for these clean energy applications requires design principles for nitride dissolution and ammonia formation in acid. Here, we report that lowering the nitrogen 2p band center of transition metal nitrides relative to the Fermi level weakens metal–nitrogen bonds and increases labile metallic character, reducing dissolution reaction barriers and boosting ammonia formation kinetics in acid. Increasing the solubility of dissolved metal cations further facilitates the decomposition of nitrides in acid by prohibiting surface oxide passivation. These findings highlight essential future directions for preventing nitride dissolution or facilitating ammonia production for diverse acidic applications.

Li–O2 batteries can provide greater gravimetric energy than Li-ion batteries but suffer from poor efficiency and cycle life due to the instability of aprotic electrolytes. In this study, we show that the apparent four-electron oxygen reduction to form Li2O in Li–O2 batteries with molten nitrate is facilitated by the electrochemical reduction of nitrate to nitrite, and subsequent chemical oxidation of nitrite to nitrate by molecular oxygen, instead of a four-electron oxygen reduction aided by disproportionation of Li2O2 generated from two-electron reduction of molecular oxygen. By examining a series of transition metal catalysts using experiments and computation, optimizing the surface binding of nitrate to enhance the kinetics of the electrochemical reduction of nitrate to nitrite, as well as increasing the kinetics of nitrite oxidation by O2 was shown to increase the discharge voltage and render the observed high-rate capability for NiO-based surfaces in Li–O2 batteries.

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