Nitrogen cold plasma treatment stabilizes Cu^(0)/Cu^(+) electrocatalysts to enhance CO_(2) to C2 conversion
作者机构:School of Chemistry&Chemical EngineeringChongqing University of TechnologyChongqing 400054China College of Biomass Science and EngineeringSichuan UniversityChengdu 610065SichuanChina Chongqing Institute of Green and Intelligent TechnologyChinese Academy of SciencesChongqing 400714China Research School of ChemistryAustralian National UniversityCanberraACT 2601Australia
出 版 物:《Journal of Energy Chemistry》 (能源化学(英文版))
年 卷 期:2023年第84卷第9期
页 面:321-328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:the National Natural Science Foundation of China (21902017) the Foundation of technological innovation and application development of Chongqing (cstc2021jscxmsxm X0308, CSTB2022BSXM-JCX0132) the Youth project of science and technology research program of Chongqing Education Commission of China (KJQN20211107) the Scientific Research Foundation of Chongqing University of Technology (2020ZDZ022, 2021PYZ13)
主 题:Nitrogen cold plasma Cu-based metal nitride Carbon dioxide electroreduction C2 products Stabilizes
摘 要:Cu-based materials are ideal catalysts for CO_(2) electrocatalytic reduction reaction(CO_(2)RR) into multicarbon ***,such reactions require stringent conditions on local environments of catalyst surfaces,which currently are the global pressing ***,a stabilized activation of Cu^(0)/Cu^(+)-onAg interface by N_(2) cold plasma treatment was developed for improving Faradaic efficiency(FE) of CO_(2)RR into C2 *** resultant Ag@Cu-CuN_x exhibits a C2 FE of 72% with a partial current density of-14.9 mA cm^(-2) at-1.0 V ***(reversible hydrogen electrode).Combining density functional theory(DFT) and experimental investigations,we unveiled that Cu^(0)/Cu^(+) species can be co ntrollably tu ned by the incorporation of nitrogen to form CuN_x on Ag surface,i.e.,Ag@Cu-CuN_*** strategy enhances ^(*)CO intermediates generation and accelerates C-C coupling both thermodynamically and *** intermediates O^(*)C^(*)CO,^(*)COOH,and ^(*)CO were detected by in-situ attenuated total internal reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS).The uncovered CO_(2)RR-into-C2 products were carried out along CO_(2)→^(*)COOH→^(*)CO→O^(*)C^(*)CO→^(*)C_(2)H_(3)O→^(*)C_(2)H_(4)O→ C_(2)H_(5)OH(or ^(*)C_(2)H_(3)O→^(*)O+C_(2)H_(4)) paths over Ag@Cu-CuN_x *** work provides a new approach to design Cu-based electrocatalysts with high-efficiency,mild condition,and stable CO_(2)RR to C2 products.