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 neutra...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.展开更多
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。
文摘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.
