张宁
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祝贺课题组在《Angewandte Chemie International Edition》上发表有关电驱动C-N偶联合成酰胺化合物的研究论文!第一作者为博士生刘振中!
Title: Directing the Electrochemical C−N Coupling towards Efficient Amide Synthesis via Ammonia Activation-Mediated Pathway
Abstract: Electrochemically oxidative C−N coupling using alcohol and ammonia as feedstocks offers a sustainable alternative for the chemosynthesis of amide organonitrogens. The achievements of high activity and selectivity yet remains challenging via the conventional alcohol oxidation pathway. Here, we present an alternative ammonia-activation mediated pathway to favor the electrochemical C−N coupling necessary. Spectroscopic and theoretical investigations untangle that this manipulated process begins with the oxidation of ammonia to endow active *NH2 species, which then efficiently couple with alcohol species to form C−N bonds. This alternative C−N coupling pathway exhibits accelerated kinetics and, more importantly, bypasses the formation of aldehyde intermediate, thereby preventing unfavorable overoxidation. As a result, this pathway achieves a high Faradaic efficiency of 50.1% and a carbon selectivity of 87.6% for efficient formamide electrosynthesis over a NiCuRu-based (oxy)hydroxide catalyst, with a productivity of 557.2 μmol cm−2 h−1. Such electrosynthetic approach further exhibit the universality of waste biomass/plastics-driven carbon feedstocks, achieving considerable Faradaic efficiencies of 32−60%. Techno-economic analysis confirms the potential profitability of using renewable electricity input, highlighting the significant advantages of green chemical manufacturing for sustainable development.
