Efficient nitrate electroreduction over Mn-doped Cu catalyst via regulating N-containing intermediates adsorption configuration  

作　　者：Limin Wu Shunhan Jia Libing Zhang Ruhan Wang Jiaqi Feng Xiaofu Sun Buxing Han 

机构地区：[1]Beijing National Laboratory for Molecular Sciences,CAS Laboratory of Colloid and Interface and Thermodynamics,CAS Research/Education Center for Excellence in Molecular Sciences,Center for Carbon Neutral Chemistry,Institute of Chemistry,Chinese Academy of Sciences,Beijing,100190,China [2]School of Chemical Sciences,University of Chinese Academy of Sciences,Beijing,100049,China [3]College of Chemical Engineering and Environment,China University of Petroleum,Beijing,102249,China [4]Shanghai Key Laboratory of Green Chemistry and Chemical Processes,School of Chemistry and Molecular Engineering,East China Normal University,Shanghai,200062,China

出　　处：《Science China Chemistry》2024年第6期1969-1975,共7页中国科学（化学英文版）

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。

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).

关 键 词：nitrate reduction ELECTROCATALYSIS ammonia synthesis N-intermediate green chemistry 

分 类 号：TQ113.2[化学工程—无机化工] TQ426