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Abstract
Electrifying chemical manufacturing using renewable energy is an attractive approach to reduce the dependence on fossil energy sources in chemical industries. Primary amines are important organic building blocks; however, the synthesis is often hindered by the poor selectivity because of the formation of secondary and tertiary amine byproducts. Herein, we report an electrocatalytic route to produce ethylamine selectively through an electroreduction of acetonitrile at ambient temperature and pressure. Among all the electrocatalysts, Cu nanoparticles exhibit the highest ethylamine Faradaic efficiency (~96%) at −0.29 V versus reversible hydrogen electrode. Under optimal conditions, we achieve an ethylamine partial current density of 846 mA cm−2. A 20-hour stable performance is demonstrated on Cu at 100 mA cm−2 with an 86% ethylamine Faradaic efficiency. Moreover, the reaction mechanism is investigated by computational study, which suggests the high ethylamine selectivity on Cu is due to the moderate binding affinity for the reaction intermediates.
Industrial synthesis of primary amine often features poor selectivity because of the formation of secondary and tertiary amine byproducts. Here, the authors report an electrocatalytic route to ethylamine through selective electroreduction of acetonitrile at ambient temperature and pressure.
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1 University of Delaware, Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, Newark, United States (GRID:grid.33489.35) (ISNI:0000 0001 0454 4791); Tianjin University, Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin, China (GRID:grid.33763.32) (ISNI:0000 0004 1761 2484)
2 Columbia University, Department of Chemical Engineering, New York, United States (GRID:grid.21729.3f) (ISNI:0000000419368729)
3 Florida A&M University, Department of Physics, Tallahassee, USA (GRID:grid.255948.7) (ISNI:0000 0001 2214 9445)
4 University of Delaware, Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, Newark, United States (GRID:grid.33489.35) (ISNI:0000 0001 0454 4791)
5 Tianjin University, Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin, China (GRID:grid.33763.32) (ISNI:0000 0004 1761 2484)