Cu-based metal-organic frameworks(Cu-MOFs)electrocatalysts are promising for CO_(2)reduction reactions(CO_(2)RR)to produce valuable C_(2+)products.However,designing suitable active sites in Cu-MOFs remains challenging...Cu-based metal-organic frameworks(Cu-MOFs)electrocatalysts are promising for CO_(2)reduction reactions(CO_(2)RR)to produce valuable C_(2+)products.However,designing suitable active sites in Cu-MOFs remains challenging due to their inherent structural instability during CO_(2)RR.Here we propose a synergistic strategy through thermal annealing and electrochemicalactivation process for in-situ reconstruction of the pre-designed Cu-MOFs to produce abundant partially oxidized Cu(Cu^(δ+))active species.The optimized MOF-derived Cu^(δ+)electrocatalyst demonstrates a highly selective production of C_(2+)products,with the Faradaic Efficiency(FE)of 78±2%and a partial current density of-46 m A cm-2at-1.06 VRHEin a standard H-type cell.Our findings reveal that the optimized Cu^(δ+)-rich surface remains stable during electrolysis and enhances surface charge transfer,leading to an increase in the concentration of*CO intermediates,thereby highly selectively producing C_(2+)compounds.This study advances the controllable formation of MOF-derived Cu^(δ+)-rich surfaces and strengthens the understanding of their catalytic role in CO_(2)RR for C_(2+)products.展开更多
基金supported by the Research Grants Council(16310419,16309418,and 16304821)the Innovation and Technology Commission(Grant No.ITC-CNERC14EG03)of the Hong Kong Special Administrative Region+4 种基金the Hong Kong Branch of National Precious Metals Material Engineering Research Centre,City University of Hong Kongthe Strategic Hiring Scheme of The Hong Kong Polytechnic University(P0047728)GuangDong Basic and Applied Basic Research Foundation(2023A1515110259)National Natural Science Foundation of China(22405228)Guangzhou Science and Technology Bureau(2024A03J0609)。
文摘Cu-based metal-organic frameworks(Cu-MOFs)electrocatalysts are promising for CO_(2)reduction reactions(CO_(2)RR)to produce valuable C_(2+)products.However,designing suitable active sites in Cu-MOFs remains challenging due to their inherent structural instability during CO_(2)RR.Here we propose a synergistic strategy through thermal annealing and electrochemicalactivation process for in-situ reconstruction of the pre-designed Cu-MOFs to produce abundant partially oxidized Cu(Cu^(δ+))active species.The optimized MOF-derived Cu^(δ+)electrocatalyst demonstrates a highly selective production of C_(2+)products,with the Faradaic Efficiency(FE)of 78±2%and a partial current density of-46 m A cm-2at-1.06 VRHEin a standard H-type cell.Our findings reveal that the optimized Cu^(δ+)-rich surface remains stable during electrolysis and enhances surface charge transfer,leading to an increase in the concentration of*CO intermediates,thereby highly selectively producing C_(2+)compounds.This study advances the controllable formation of MOF-derived Cu^(δ+)-rich surfaces and strengthens the understanding of their catalytic role in CO_(2)RR for C_(2+)products.
