Unraveling the Dynamic Structural Evolution of Phthalocyanine Catalysts during CO_(2) Electroreduction  

作　　者：Jianing Mao Bingbao Mei Ji Li Shuai Yang Fanfei Sun Siyu Lu Wei Chen Fei Song Zheng Jiang 

机构地区：[1]Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201204,China [2]University of Chinese Academy of Sciences,Beijing 100049,China [3]Shanghai Synchrotron Radiation Facility,Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai 201204,China [4]College of Chemistry,College of Materials Science and Engineering,Zhengzhou University,Zhengzhou 450000,China [5]Low-Carbon Conversion Science and Engineering Center,Shanghai Advanced Research Institute,Chinese Academy of Science,Shanghai 201210,China [6]Innovation Academy for Green Manufacture,Chinese Academy of Sciences,Bejing 100190,China

出　　处：《Chinese Journal of Structural Chemistry》2022年第10期82-88,共7页结构化学（英文）

基　　金：supported by the National Natural Science Foundation of China (U1732267);Shanghai Science and Technology Development Funds (22YF1454500);Photon Science Center for Carbon Neutrality and Low-Carbon Conversion Science and Engineering Center。

摘　　要：Understanding the atomic and electronic changes of active sites promotes the whole new sight into electrochemical carbon dioxide reduction reaction(CO_(2)RR),which provides a feasible strategy to achieve carbon neutrality.Here we employ operando high-energy resolution fluorescence-detected Xray absorption spectroscopy(HERFD-XAS)to track the structural evolution of Ni(II)phthalocyanine(NiPc),considered as the model catalysts with uniform Ni-N_(4)-C_(8) moiety,during the CO_(2)RR.The HERFD-XAS method is in favor of elucidating the interaction of the reactant/catalyst interface from the atomic electronic structure dimension,facilitating the establishment of the catalytic mechanism and the dynamic structure changes.Based on operando measurement,surface sensitive difference spectra(△μ)and spectroscopy simulation,the interfacial interactions between the active sites of NiPc and reactants are monitored and the Ni species gradually reduced by increasing the applied potential is discovered.HERFD-XAS method offers an advanced and powerful tool for elucidating the complex catalytic mechanism in further various systems.

关 键 词：CO_(2)electrochemical reduction HERFD-XAS model catalysts difference spectra structural evolution 

分 类 号：TQ426[化学工程] X701[环境科学与工程—环境工程]