Atomic-Scale Tailoring C–N Coupling Sites for Efficient Acetamide Electrosynthesis over Cu-Anchored Boron Nitride Nanosheets

作者：Yan Wang, Shuai Xia, Kui Chen, Jianfang Zhang, Hao Tan, Cuiping Yu, Jiewu Cui, Jianrong Zeng, Jingjie Wu, Peng Wang, Yucheng Wu · 发表于：ACS Nano · 年份：2024 · DOI：10.1021/acsnano.4c14039 · 被引用次数：66 · 研究领域：Asymmetric Hydrogenation and Catalysis、Ammonia Synthesis and Nitrogen Reduction、Covalent Organic Framework Applications

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.