Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis,but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging.Herein,we ...Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis,but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging.Herein,we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts,named FeNi@nC-T(n represents the content of nanoporous carbon as 1,3,5,7 or 9 g and T=900,950,1000 or 1100°C),for highly performed urea synthesis via NO_(3)−and CO_(2)co-reduction.The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h^(−1)gFeNi^(−1)with a Faradaic efficiency of 15.56%at–1.2 V vs.RHE.Moreover,the scale-up synthesized FeNi@7C-950-S(over 140 g per batch)was achieved with its high catalytic performance and high stability maintained.Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key*CO and*N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.展开更多
文摘Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis,but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging.Herein,we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts,named FeNi@nC-T(n represents the content of nanoporous carbon as 1,3,5,7 or 9 g and T=900,950,1000 or 1100°C),for highly performed urea synthesis via NO_(3)−and CO_(2)co-reduction.The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h^(−1)gFeNi^(−1)with a Faradaic efficiency of 15.56%at–1.2 V vs.RHE.Moreover,the scale-up synthesized FeNi@7C-950-S(over 140 g per batch)was achieved with its high catalytic performance and high stability maintained.Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key*CO and*N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.
基金Project supported by the National Natural Science Foundation of China(No.51275453)the Key Research Project of Lishui,China(No.2016ZDYF15)the North Vehicle Research Institute,and Hangzhou Advance Gearbox Group Co.,Ltd.,China