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 

作者机构：Beijing National Laboratory for Molecular SciencesCAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of Chemical SciencesUniversity of Chinese Academy of SciencesBeijing100049China College of Chemical Engineering and EnvironmentChina University of PetroleumBeijing102249China Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai200062China 

出 版 物：《Science China Chemistry》 (中国科学（化学英文版）)

年 卷 期：2024年第67卷第6期

页      面：1969-1975页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

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 

主　　题：nitrate reduction electrocatalysis ammonia synthesis N-intermediate green chemistry 

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 ***,challenges exist due to its sluggish kinetics,multiple intermediates,and various reaction *** this study,Mn-doped-Cu catalyst was synthesized and employed for electrochemical NO_(3)^(-)-to-NH_(3)*** 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)^(-)*** 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**** alteration decreased the energy barrier of*NO-to-*NOH,consequently promoting the conversion of NO_(3)^(-)-to-NH_(3).