Earth-abundant and nontoxic Sn-based materials have been regarded as promising catalysts for the electrochemical conversion of CO_(2)to C1 products,e.g.,CO and formate.However,it is still difficult for Snbased materia...Earth-abundant and nontoxic Sn-based materials have been regarded as promising catalysts for the electrochemical conversion of CO_(2)to C1 products,e.g.,CO and formate.However,it is still difficult for Snbased materials to obtain satisfactory performance at low-to-moderate overpotentials.Herein,a simple and facile electrospinning technique is utilized to prepare a composite of a bimetallic Sn-Co oxide/carbon matrix with a hollow nanotube structure(Sn Co-HNT).Sn Co-HNT can maintain>90%faradaic efficiencies for C1 products within a wide potential range from-0.6 VRHE to-1.2 VRHE,and a highest 94.1%selectivity towards CO in an H-type cell.Moreover,a 91.2%faradaic efficiency with a 241.3 m A cm^(-2)partial current density for C1 products could be achieved using a flow cell.According to theoretical calculations,the fusing of Sn/Co oxides on the carbon matrix accelerates electron transfer at the atomic level,causing electron deficiency of Sn centers and reversible variation between Co^(2+)and Co^(3+)centers.The synergistic effect of the Sn/Co composition improves the electron affinity of the catalyst surface,which is conducive to the adsorption and stabilization of key intermediates and eventually increases the catalytic activity in CO_(2)electroreduction.This study could provide a new strategy for the construction of oxide-derived catalysts for CO_(2)electroreduction.展开更多
To realize the goal of carbon peaking and carbon neutrality,CO_(2) capture and utilization technology is becoming increasingly urgent.However,the low efficiency and complex processes limit its large-scale application....To realize the goal of carbon peaking and carbon neutrality,CO_(2) capture and utilization technology is becoming increasingly urgent.However,the low efficiency and complex processes limit its large-scale application.Among utilization technology of CO_(2),electrochemical CO_(2) reduction reaction(CO_(2)RR)has attracted interest,attributing to the use of clean energy and the final product of value-added fuels.The construction of catalysts with integrated CO_(2) capture and reduction ability is expected to bridge the gap between CO_(2) capture and conversion,achieving the direct utilization of flue gas,reducing costs,and simplifying devices.Keeping` this in mind,we give this review to introduce the problems of lowconcentration CO_(2)RR and the significance of coupled CO_(2) capture/conversion electrocatalysts in addressing the emission of industrial flue gas first.Then,the regulation strategies,including functional group modification,co-catalytic effect,and catalysts-impurities interaction,which affected the CO_(2) capture and electroreduction capacity towards catalysts were summarized and discussed.Finally,the challenges and perspectives about the design for linked CO_(2) capture/conversion processes were proposed.This review will provide new insight into the building of multifunctional catalysts for CO_(2) conversion.展开更多
基金supported by the National Natural Science Foundation of China(U21A20312,22172099,21975162,51902209)the Natural Science Foundation of Guangdong(2020A1515010840)the Shenzhen Science and Technology Program(SGDX20201103095802006,RCBS20200714114819161,JCYJ20190808111801674,JCYJ20200109105803806,RCYX20200714114535052)。
文摘Earth-abundant and nontoxic Sn-based materials have been regarded as promising catalysts for the electrochemical conversion of CO_(2)to C1 products,e.g.,CO and formate.However,it is still difficult for Snbased materials to obtain satisfactory performance at low-to-moderate overpotentials.Herein,a simple and facile electrospinning technique is utilized to prepare a composite of a bimetallic Sn-Co oxide/carbon matrix with a hollow nanotube structure(Sn Co-HNT).Sn Co-HNT can maintain>90%faradaic efficiencies for C1 products within a wide potential range from-0.6 VRHE to-1.2 VRHE,and a highest 94.1%selectivity towards CO in an H-type cell.Moreover,a 91.2%faradaic efficiency with a 241.3 m A cm^(-2)partial current density for C1 products could be achieved using a flow cell.According to theoretical calculations,the fusing of Sn/Co oxides on the carbon matrix accelerates electron transfer at the atomic level,causing electron deficiency of Sn centers and reversible variation between Co^(2+)and Co^(3+)centers.The synergistic effect of the Sn/Co composition improves the electron affinity of the catalyst surface,which is conducive to the adsorption and stabilization of key intermediates and eventually increases the catalytic activity in CO_(2)electroreduction.This study could provide a new strategy for the construction of oxide-derived catalysts for CO_(2)electroreduction.
基金financially supported by the National Natural Science Foundation of China(No.22273093)the CAS Project for Young Scientists in Basic Re-search(YSBR-005)the start-up funding of University of Science and Technology of China。
文摘To realize the goal of carbon peaking and carbon neutrality,CO_(2) capture and utilization technology is becoming increasingly urgent.However,the low efficiency and complex processes limit its large-scale application.Among utilization technology of CO_(2),electrochemical CO_(2) reduction reaction(CO_(2)RR)has attracted interest,attributing to the use of clean energy and the final product of value-added fuels.The construction of catalysts with integrated CO_(2) capture and reduction ability is expected to bridge the gap between CO_(2) capture and conversion,achieving the direct utilization of flue gas,reducing costs,and simplifying devices.Keeping` this in mind,we give this review to introduce the problems of lowconcentration CO_(2)RR and the significance of coupled CO_(2) capture/conversion electrocatalysts in addressing the emission of industrial flue gas first.Then,the regulation strategies,including functional group modification,co-catalytic effect,and catalysts-impurities interaction,which affected the CO_(2) capture and electroreduction capacity towards catalysts were summarized and discussed.Finally,the challenges and perspectives about the design for linked CO_(2) capture/conversion processes were proposed.This review will provide new insight into the building of multifunctional catalysts for CO_(2) conversion.
