Operando HERFD-XANES and surface sensitive Δμ analyses identify the structural evolution of copper(Ⅱ) phthalocyanine for electroreduction of CO_(2)

作     者：Bingbao Mei Cong Liu Ji Li Songqi Gu Xianlong Du Siyu Lu Fei Song Weilin Xu Zheng Jiang Bingbao Mei;Cong Liu;Ji Li;Songqi Gu;Xianlong Du;Siyu Lu;Fei Song;Weilin Xu;Zheng Jiang

作者机构：Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201204China University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Electroanalytical Chemistry&Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina Shanghai Synchrotron Radiation FacilityShanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China College of ChemistryCollege of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450000HenanChina Innovation Academy for Green ManufactureChinese Academy of SciencesBeijing 100190China 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2022年第31卷第1期

页      面：1-7,I0001页

核心收录：

学科分类：0820[工学-石油与天然气工程] 0808[工学-电气工程] 081704[工学-应用化学] 081705[工学-工业催化] 07[理学] 0817[工学-化学工程与技术] 08[工学] 0807[工学-动力工程及工程热物理] 070302[理学-分析化学] 0827[工学-核科学与技术] 0703[理学-化学] 

基　　金：supported by the National Natural Science Foundation of China grant number:U1732267 

主　　题：Operando HERFD-XANES △μanalysis Structural evolution Copper(Ⅱ)phthalocyanine Electrochemical CO_(2)reduction reaction 

摘      要：The quantitative understanding of how atomic-level catalyst structural changes affect the reactivity of the electrochemical CO_(2)reduction reaction is *** to the complexity of catalytic systems,conventional in situ X-ray spectroscopy plays a limited role in tracing the underlying dynamic structural changes in catalysts active ***,operando high-energy resolution fluorescence-detected X-ray absorption spectroscopy was used to precisely identify the dynamic structural transformation of well-defined active sites of a representative model copper(Ⅱ)phthalocyanine catalyst which is of guiding significance in studying single-atom catalysis *** X-ray spectroscopy analyses,including surface sensitive△μspectra which isolates the surface changes by subtracting the disturb of bulk base and X-ray absorption near-edge structure spectroscopy simulation,were used to discover that Cu species aggregated with increasing applied potential,which is responsible for the observed evolution of C_(2)H_(4).The approach developed in this work,characterizing the active-site geometry and dynamic structural change,is a novel and powerful technique to elucidate complex catalytic mechanisms and is expected to con tribute to the rational design of highly effective catalysts.