Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO_(2)reduction reaction(CO_(2)RR)toward multi-carbon(C2+)products,primarily by suppressing the pa...Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO_(2)reduction reaction(CO_(2)RR)toward multi-carbon(C2+)products,primarily by suppressing the parasitic hydrogen evolution reaction and facilitating a localized CO_(2)/CO concentration at the electrode.Building upon this approach,we developed surface-functionalized catalysts with exceptional activity and selectivity for electrocatalytic CO_(2)RR to C_(2+)in a neutral electrolyte.Employing CuO nanoparticles coated with hexaethynylbenzene organic molecules(HEB-CuO NPs),a remarkable C_(2+)Faradaic efficiency of nearly 90%was achieved at an unprecedented current density of 300 mA cm^(-2),and a high FE(>80%)was maintained at a wide range of current densities(100-600 mA cm^(-2))in neutral environments using a flow cell.Furthermore,in a membrane electrode assembly(MEA)electrolyzer,86.14%FEC2+was achieved at a partial current density of 387.6 mA cm^(-2)while maintaining continuous operation for over 50 h at a current density of 200 mA cm^(-2).In-situ spectroscopy studies and molecular dynamics simulations reveal that reducing the coverage of coordinated K⋅H2O water increased the probability of intermediate reactants(CO)interacting with the surface,thereby promoting efficient C-C coupling and enhancing the yield of C_(2+)products.This advancement offers significant potential for optimizing local micro-environments for sustainable and highly efficient C_(2+)production.展开更多
基金supported by the National Natural Science Foundation of China(22101182)the Shenzhen Science and Technology Program(Nos.JCYJ20210324095202006,JCYJ20220531095813031,and JCYJ20230807140700001)Guangdong Basic and Applied Basic Research Foundation(2022A1515010318).
文摘Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO_(2)reduction reaction(CO_(2)RR)toward multi-carbon(C2+)products,primarily by suppressing the parasitic hydrogen evolution reaction and facilitating a localized CO_(2)/CO concentration at the electrode.Building upon this approach,we developed surface-functionalized catalysts with exceptional activity and selectivity for electrocatalytic CO_(2)RR to C_(2+)in a neutral electrolyte.Employing CuO nanoparticles coated with hexaethynylbenzene organic molecules(HEB-CuO NPs),a remarkable C_(2+)Faradaic efficiency of nearly 90%was achieved at an unprecedented current density of 300 mA cm^(-2),and a high FE(>80%)was maintained at a wide range of current densities(100-600 mA cm^(-2))in neutral environments using a flow cell.Furthermore,in a membrane electrode assembly(MEA)electrolyzer,86.14%FEC2+was achieved at a partial current density of 387.6 mA cm^(-2)while maintaining continuous operation for over 50 h at a current density of 200 mA cm^(-2).In-situ spectroscopy studies and molecular dynamics simulations reveal that reducing the coverage of coordinated K⋅H2O water increased the probability of intermediate reactants(CO)interacting with the surface,thereby promoting efficient C-C coupling and enhancing the yield of C_(2+)products.This advancement offers significant potential for optimizing local micro-environments for sustainable and highly efficient C_(2+)production.
