Atomic-Scale\nTailoring C–N Coupling Sites for\nEfficient Acetamide Electrosynthesis over Cu-Anchored Boron Nitride\nNanosheets

Electrochemical\nconversion of carbon and nitrogen sources into\nvaluable chemicals provides a promising strategy for mitigating CO<sub>2</sub> emissions and tackling pollutants. However, efficiently scaling\nup C–N products beyond basic compounds like urea remains a\nsignificant challenge. Herein, we upgrade the C–N coupling\nfor acetamide synthesis through coreducing CO and nitrate (NO<sub>3</sub><sup>–</sup>) on atomic-scale Cu dispersed on boron\nnitride (Cu/BN) nanosheets. The specific form of Cu, such as single\natom, nanocluster, and nanoparticles, endows Cu/BN different adsorption\ncapacity for CO and NO<sub>3</sub><sup>–</sup>, thereby dictating\nthe catalytic activity and selectivity for acetamide formation. The\nCu nanocluster-anchored BN (Cu NCs/BN) catalyst achieves an industrial-level\ncurrent density of 178 mA cm<sup>–2</sup> for the C–N\ncoupling reaction and an average acetamide yield rate of 137.0 mmol\nh<sup>–1</sup> g<sub>cat.</sub><sup>–1</sup> at −1.6\nV versus the reversible hydrogen electrode. Experimental and theoretical\nanalyses uncover the pivotal role of the strong electronic interaction\nbetween Cu nanoclusters and BN, which activates CO and NO<sub>3</sub><sup>–</sup>, facilitates the formation of key *CCO and *NH<sub>2</sub> intermediates, and expedites the C–N coupling pathway\nto acetamide. This work propels the development of atomic structure\ncatalysts for the efficient conversion of small molecules to high-value\nchemicals through electrochemical processes.