摘要
The electrochemical reduction of NO_(3)^(-)to NH_(3)holds promise for economic and environmental benefits,presenting an energyefficient alternative to the traditional Haber-Bosch method.However,challenges exist due to its sluggish kinetics,multiple intermediates,and various reaction pathways.In this study,Mn-doped-Cu catalyst was synthesized and employed for electrochemical NO_(3)^(-)-to-NH_(3)conversion.The doping of Mn into Cu resulted in exceptional performance,achieving a FE of 95.8%and an NH_(3)yield rate of 0.91 mol g^(-1)h^(-1)at-0.6 V in a neutral electrolyte at low NO_(3)^(-)concentration.Detailed experimental studies and theoretical calculations revealed that the Mn dopant enhanced the kinetic rate of NO_(2)~--to-NH_(3)and induced a distinct configuration of*NO.This alteration decreased the energy barrier of*NO-to-*NOH,consequently promoting the conversion of NO_(3)^(-)-to-NH_(3).
基金
supported by the National Natural Science Foundation of China(22293015,22203099,and 22121002)
Strategic Priority Research Program(A)of the Chinese Academy of Sciences(XDA0390400)
Photon Science Center for Carbon Neutrality。