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Electrochemical conversion of carbon and nitrogen sources into valuable chemicals provides a promising strategy for mitigating CO 2 emissions and tackling pollutants. However, efficiently scaling up C–N products beyond basic compounds like urea remains a significant challenge. Herein, we upgrade the C–N coupling for acetamide synthesis through coreducing CO and nitrate (NO 3 – ) on atomic-scale Cu dispersed on boron nitride (Cu/BN) nanosheets. The specific form of Cu, such as single atom, nanocluster, and nanoparticles, endows Cu/BN different adsorption capacity for CO and NO 3 –, thereby dictating the catalytic activity and selectivity for acetamide formation. The Cu nanocluster-anchored BN (Cu NCs/BN) catalyst achieves an industrial-level current density of 178 mA cm –2 for the C–N coupling reaction and an average acetamide yield rate of 137.0 mmol h –1 g cat. –1 at −1.6 V versus the reversible hydrogen electrode. Experimental and theoretical analyses uncover the pivotal role of the strong electronic interaction between Cu nanoclusters and BN, which activates CO and NO 3 –, facilitates the formation of key *CCO and *NH 2 intermediates, and expedites the C–N coupling pathway to acetamide. This work propels the development of atomic structure catalysts for the efficient conversion of small molecules to high-value chemicals through electrochemical processes.
Wang et al. (Wed,) studied this question.