Two-Dimensional MOF\nConstructed by a Binuclear-Copper\nMotif for High-Performance Electrocatalytic NO Reduction to NH<sub>3</sub>

Ambient electrochemical\nNO reduction presents a dual\nsolution for\nsustainable NO reduction and NH<sub>3</sub> synthesis. However, their\ncomplex kinetics and energy demands necessitate high-performance electrocatalysts\nto ensure effective and selective process outcomes. Herein, we report\nthat a two-dimensional Cu-based metal–organic framework (MOF),\n{[Cu(HL)]·H<sub>2</sub>O}<sub><i>n</i></sub>, (<b>Cu-OUC</b>, H<sub>3</sub>L = 5-(2′-carboxylphenoxy)isophthalic\nacid) acts as a stable electrocatalyst with high efficiency for NO-to-NH<sub>3</sub> conversion. Electrochemical experimental studies showed that\nin 0.1 M K<sub>2</sub>SO<sub>4</sub> solution, the as-prepared <b>Cu-OUC</b> achieved a peak Faradaic efficiency of 96.91% and a\nnotable NH<sub>3</sub> yield as high as 3415.82 μg h<sup>–1</sup> mg<sup>–1</sup>. The Zn–NO battery in aqueous solution\ncan produce electricity possessing a power density of 2.04 mW cm<sup>–2</sup> while simultaneously achieving an NH<sub>3</sub> yield\nof 616.92 μg h<sup>–1</sup> mg<sup>–1</sup>. Theoretical\ncalculations revealed that the surface of <b>Cu-OUC</b> effectively\nfacilitates NO activation through a two-way charge transfer mechanism\nof “electron acceptance and donation”, with the *NO\nformation step being the potential-determining stage. The study pioneers\nthe use of a MOF as an electrocatalyst for ambient NO-to-NH<sub>3</sub> conversion.