Activation of Transition Metal(Fe,Co and Ni)-Oxide Nanoclusters by Nitrogen Defects in Carbon Nanotube for Selective CO_(2) Reduction Reaction

作     者：Yi Cheng Jinfan Chen Chujie Yang Huiping Wang Bernt Johannessen Lars Thomsen Martin Saunders Jianping Xiao Shize Yang San Ping Jiang Yi Cheng;Jinfan Chen;Chujie Yang;Huiping Wang;Bernt Johannessen;Lars Thomsen;Martin Saunders;Jianping Xiao;Shize Yang;San Ping Jiang

作者机构：Institute of Environmental Science and EngineeringSchool of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China Institute of MaterialsChina Academy of Engineering PhysicsP.O.Box 9071-12Mianyang 621907China Australian SynchrotronANSTOClayton Vic.3168Australia Centre for MicroscopyCharacterization and Analysis(CMCA)The University of Western AustraliaCrawley WA 6009Australia State Key Laboratory of CatalysisDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Eyring Materials CenterArizona State UniversityTempe AZ 85257USA WA School of Mines:MineralsEnergy&Chemical EngineeringCurtin UniversityPerth WA 6102Australia 

出 版 物：《Energy & Environmental Materials》 (能源与环境材料（英文）)

年 卷 期：2023年第6卷第1期

页      面：253-263页

核心收录：

学科分类：0710[理学-生物学] 0830[工学-环境科学与工程（可授工学、理学、农学学位）] 08[工学] 0807[工学-动力工程及工程热物理] 0815[工学-水利工程] 0706[理学-大气科学] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 0702[理学-物理学] 

基　　金：Y.C.and J.C.are contributed equally to the paper.Project supported by the National Natural Science Foundation of China (U19A2017) the Fundamental Research Funds for the Central South University and the Australian Research Council (DP180100731 and DP180100568) 

主　　题：activation effect electrochemical CO_(2)reduction reaction N defect proton-coupled electron transfer process transition metal oxide nanocluster 

摘      要：The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish ***,highly efficient,cheap catalysts are urgently *** metal oxides such as CoO_(x),FeO_(x),and NiO_(x)are low-cost,low toxicity,and abundant materials for a wide range of electrochemical reactions,but are almost inert for CO_(2)***,we report for the first time that nitrogen doped carbon nanotubes(N-CNT)have a surprising activation effect on the activity and selectivity of transition metal-oxide(MO_(x)where M=Fe,Ni,and Co)nanoclusters for CO_(2)***_(x)supported on N-CNT,MO_(x)/N-CNT,achieves a CO yield of 2.6–2.8 mmol cm−2 min−1 at an overpotential of−0.55 V,which is two orders of magnitude higher than MO_(x)supported on acid treated CNTs(MO_(x)/O-CNT)and four times higher than pristine *** faraday efficiency for electrochemical CO_(2)-to-CO conversion is as high as 90.3%at overpotential of 0.44 *** in-situ XAS measurements and DFT calculations disclose that MO_(x)nanoclusters can be hydrated in CO_(2)saturated KHCO_(3),and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions,which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions.