The electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to obtain valuable chemicals is an appealing way to ease the energy and environmental crises,but the development of efficient catalysts remains challenging.Herein...The electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to obtain valuable chemicals is an appealing way to ease the energy and environmental crises,but the development of efficient catalysts remains challenging.Herein,we report a novel Ag-MnO_(x)heterostructured catalyst and its high activity for the CO_(2)RR to CO.The obtained Ag-MnO_(x)exhibits a CO faradaic efficiency(FECO)of up to 97.5%at-0.8 V vs.reversible hydrogen electrode(RHE)and especially maintains an FECO above 90%within a broad potential window of 500 mV(-0.6 to-1.1 V vs.RHE).In addition,the CO_(2)RR performance was optimized using a flow cell,and the Ag-MnO_(x)catalyst reached a total current density of-255 mA cm^(-2)at-2.0 V vs.RHE.Our designed in situ experiments and density functional theory(DFT)calculations reveal that the heterojunction interface formed between O-defect-rich MnO_(x)and active Ag enhances CO_(2)adsorption and activation and simultaneously stabilizes the*COOH intermediate,thus leading to its superior catalytic performance.Furthermore,the Ag-MnO_(x)catalyst used as the cathode to assemble a Zn-CO_(2)cell exhibited an ultimate power density of 13.63 mW cm^(-2)and recharge time of over 65 h.展开更多
基金support from the National Natural Science Foundation of China(Grant No.52401038)Guangxi Science and Technology Program[No.Guike AD23026107]Natural Science Foundation of Guangxi Province of China[No.2024GXNSFBA010234].
文摘The electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to obtain valuable chemicals is an appealing way to ease the energy and environmental crises,but the development of efficient catalysts remains challenging.Herein,we report a novel Ag-MnO_(x)heterostructured catalyst and its high activity for the CO_(2)RR to CO.The obtained Ag-MnO_(x)exhibits a CO faradaic efficiency(FECO)of up to 97.5%at-0.8 V vs.reversible hydrogen electrode(RHE)and especially maintains an FECO above 90%within a broad potential window of 500 mV(-0.6 to-1.1 V vs.RHE).In addition,the CO_(2)RR performance was optimized using a flow cell,and the Ag-MnO_(x)catalyst reached a total current density of-255 mA cm^(-2)at-2.0 V vs.RHE.Our designed in situ experiments and density functional theory(DFT)calculations reveal that the heterojunction interface formed between O-defect-rich MnO_(x)and active Ag enhances CO_(2)adsorption and activation and simultaneously stabilizes the*COOH intermediate,thus leading to its superior catalytic performance.Furthermore,the Ag-MnO_(x)catalyst used as the cathode to assemble a Zn-CO_(2)cell exhibited an ultimate power density of 13.63 mW cm^(-2)and recharge time of over 65 h.
