The electrochemical CO_(2)reduction reaction(ECO_(2)RR)to formate is perceived as a technoeconomic pathway for transforming renewable electricity into fuels.However,the indeterminate mechanism underlying structural se...The electrochemical CO_(2)reduction reaction(ECO_(2)RR)to formate is perceived as a technoeconomic pathway for transforming renewable electricity into fuels.However,the indeterminate mechanism underlying structural self-reconstruction obstructs the strategic design of a high-performance In catalyst for the ECO_(2)RR.In this study,we chose InOOH as the model catalyst to illustrate the dynamic structure of In-based catalysts during reconstruction in the ECO_(2)RR.The findings of the current study indicate that the in situ electrochemical reconstruction of crystalline InOOH results in the creation of crystalline In clusters/InOOH,followed by In/InOOH heterostructures,and finally,metallic In over time.The efficiencies of the different phases conformed to the sequence:In clusters/InOOH>In/InOOH heterostructures>metallic In.This progression leads to a continuous drop in maximum current density and Faradaic efficiency from 29.6 mA/cm2 and 87%to 6.3 mA/cm^(2) and 75%,respectively with time extending to 7200 s,at-1.0 V relative to the reversible hydrogen electrode.Our in situ characterization and theoretical studies highlighted the crucial role of the In-cluster/InOOH interface in CO_(2)activation and conversion.展开更多
基金supported by the National Natural Science Foundation of China[22006044]External Cooperation Program of Science and Technology Planning of Fujian Province[2023I0018]+1 种基金National Engineering Laboratory for Mobile Source Emission Control Technology[NELMS2020A03]Scientific Research Funds of Huaqiao University[605-50Y200270001].
文摘The electrochemical CO_(2)reduction reaction(ECO_(2)RR)to formate is perceived as a technoeconomic pathway for transforming renewable electricity into fuels.However,the indeterminate mechanism underlying structural self-reconstruction obstructs the strategic design of a high-performance In catalyst for the ECO_(2)RR.In this study,we chose InOOH as the model catalyst to illustrate the dynamic structure of In-based catalysts during reconstruction in the ECO_(2)RR.The findings of the current study indicate that the in situ electrochemical reconstruction of crystalline InOOH results in the creation of crystalline In clusters/InOOH,followed by In/InOOH heterostructures,and finally,metallic In over time.The efficiencies of the different phases conformed to the sequence:In clusters/InOOH>In/InOOH heterostructures>metallic In.This progression leads to a continuous drop in maximum current density and Faradaic efficiency from 29.6 mA/cm2 and 87%to 6.3 mA/cm^(2) and 75%,respectively with time extending to 7200 s,at-1.0 V relative to the reversible hydrogen electrode.Our in situ characterization and theoretical studies highlighted the crucial role of the In-cluster/InOOH interface in CO_(2)activation and conversion.
