Electrocatalytic CO_(2) reduction to C2H4supplies an economically viable route for CO_(2) fixation with the integration of intermittent renewable energy.Cu-based catalysts are capable of catalyzing CO_(2) to C_(2)H_(4...Electrocatalytic CO_(2) reduction to C2H4supplies an economically viable route for CO_(2) fixation with the integration of intermittent renewable energy.Cu-based catalysts are capable of catalyzing CO_(2) to C_(2)H_(4),while suffering from the high overpotential and low Faradaic efficiency.In this joint experimentalcomputational work,an Ag-assisted carbon-carbon coupling is exploited on Cu-based catalysts.A systematic characterization analysis suggests that an ultralow quantity of Ag atoms in the Cu catalysts motivates electron transfer from Cu to Ag,regulating the electronic state of highly dispersed Ag.Meanwhile,the Ag incorporation provokes the formation of more oxygen defects on the catalyst surface,improving the adsorption and activation of CO_(2) molecules.Density functional theory studies prove the improvement effect of Ag for CO_(2)to COOH^(*).^(*)CO hydrogenation is energetically more favorable than^(*)CO dimerization pathway,and two^(*)CHO dimerization produces^(*)OCHCHO^(*) key intermediates,which greatly reduces the energy barrier for C_(2)H_(4) formation.展开更多
基金supported financially by the National Natural Science Foundation of China(21968020)the Natural Science Foundation of Inner Mongolia(2022MS02011)the Science and Technology Projects of China Northern Rare Earth(BFXT-2022-D-0023)。
文摘Electrocatalytic CO_(2) reduction to C2H4supplies an economically viable route for CO_(2) fixation with the integration of intermittent renewable energy.Cu-based catalysts are capable of catalyzing CO_(2) to C_(2)H_(4),while suffering from the high overpotential and low Faradaic efficiency.In this joint experimentalcomputational work,an Ag-assisted carbon-carbon coupling is exploited on Cu-based catalysts.A systematic characterization analysis suggests that an ultralow quantity of Ag atoms in the Cu catalysts motivates electron transfer from Cu to Ag,regulating the electronic state of highly dispersed Ag.Meanwhile,the Ag incorporation provokes the formation of more oxygen defects on the catalyst surface,improving the adsorption and activation of CO_(2) molecules.Density functional theory studies prove the improvement effect of Ag for CO_(2)to COOH^(*).^(*)CO hydrogenation is energetically more favorable than^(*)CO dimerization pathway,and two^(*)CHO dimerization produces^(*)OCHCHO^(*) key intermediates,which greatly reduces the energy barrier for C_(2)H_(4) formation.
