The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject.Cu-based bimetallic catalysts are extremely promising for efficient CO2 red...The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject.Cu-based bimetallic catalysts are extremely promising for efficient CO2 reduction.In this work,we synthesize a series of porous bimetallic Cu–Sb alloys with different compositions for the catalytic reduction of CO2 to C2H4.It is demonstrated that the alloy catalysts are much more efficient than the pure Cu catalyst.The performance of the alloy catalysts depended strongly on the composition.Further,the alloy with a Cu:Sb ratio of 10:1 yielded the best results;it exhibited a high C2H4 Faradaic efficiency of 49.7%and a high current density of 28.5 mA cm?2 at?1.19 V vs.a reversible hydrogen electrode(RHE)in 0.1 M KCl solution.To the best of our knowledge,the electrocatalytic reduction of CO2 to C2H4 using Cu–Sb alloys as catalysts has not been reported.The excellent performance of the porous alloy catalyst is attributed to its favorable electronic configuration,large surface area,high CO2 adsorption rate,and fast charge transfer rate.展开更多
The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is critical.Here,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the el...The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is critical.Here,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the electroreduction of related metallic oxides in quaternary ammonium surfactant solutions.Compared to their physical adsorption,cations embedded into the electrodes have a more pronounced impact on the electrical field,which effectively influences the adsorption state of intermediates.With the increase of surface field,the hydrogen evolution reaction and*COOH route are significantly reduced,favouring the*OCHO pathway instead.As a result,hydrogen,CO,and C_(2+)products almost completely vanish at−0.5 V versus RHE in 0.1 M Na_(2)SO_(4)in an H-type cell after enough cations are embedded into the Cu electrode,and the faradaic efficiency of formate rises from 18.0%to 99.5%simultaneously.展开更多
Electrochemical reduction of CO_2 to CO is an interesting topic. In this work, we prepared metal-free electrodes by depositing graphene oxide(GO), multi-walled carbon nanotube(MWCNT), and GO/MWCNT composites on carbon...Electrochemical reduction of CO_2 to CO is an interesting topic. In this work, we prepared metal-free electrodes by depositing graphene oxide(GO), multi-walled carbon nanotube(MWCNT), and GO/MWCNT composites on carbon paper(CP) using electrophoretic deposition(EPD) method. The electrodes were characterized by different methods, such as X-ray diffraction(XRD) and X-ray photoelectron spectroscopy(XPS). The electrochemical reduction of CO_2 to CO was conducted on the electrodes in 1-butyl-3-methylimidazolium tetrafluoroborate([Bmim]BF4)/acetonitrile(Me CN) electrolyte, and the composition of the electrolyte influenced the reaction significantly. It was demonstrated that GO/MWCNT-CP electrode was very effective for the reaction in IL(90 wt%)/Me CN binary mixture, the Faradaic efficiency of CO and current density were even higher than those on Au and Ag electrodes in the same electrolyte.展开更多
Copper(Cu)is recognized as one of the most efficient metal catalysts that can perform the electrocatalytic CO_(2) reduction reaction(CO_(2)RR)and its surface oxidation state determines the reaction pathway.The Cuδ+(0...Copper(Cu)is recognized as one of the most efficient metal catalysts that can perform the electrocatalytic CO_(2) reduction reaction(CO_(2)RR)and its surface oxidation state determines the reaction pathway.The Cuδ+(0<δ<1)species,are well known active sites in CO_(2)RR to produce hydrocarbons and oxygenates.However,Cuδ+active sites are difficult to control,and it is very easy to be reduced to Cu^(0) under CO_(2)RR operating conditions.Herein,we report a homo-hetero doping strategy to construct an efficient samarium(Sm)and sulfur(S)co-doping catalyst(Smx-CuSy)for CO_(2)RR to formic acid(HCOOH).At optimum conditions,Smx-CuSy delivered a high HCOOH Faradaic efficiency(FE)of 92.1%at the current density of 300 mA·cm^(–2) using 1 mol/L KOH aqueous solution as electrolyte,and the reduction potential was as low as–0.52 V vs.reversible hydrogen electrode(RHE).The co-doping of Sm and S resulted in excellent CO_(2)RR performance owing to the synergistic effect of the homo-hetero structure.The homo-doping of S could effectively adjust the electronic structure of Cu in favor of the formation of abundant Cu^(δ+)species.The existence of hetero-Sm species could not only stabilize the Cu^(δ+)sites,but also increase the concentration of H ions to form a favorable catalytic environment for HCOOH generation.展开更多
Electrocatalytic reduction of CO_2 is a promising route for energy storage and utilization. Herein we synthesized SnO_2 nanosheets and supported them on N-doped porous carbon (N-PC) by electrodeposition for the first ...Electrocatalytic reduction of CO_2 is a promising route for energy storage and utilization. Herein we synthesized SnO_2 nanosheets and supported them on N-doped porous carbon (N-PC) by electrodeposition for the first time. The SnO_2 and N-PC in the SnO_2@N-PC composites had exellent synergistic effect for electrocatalytic reduction of CO_2 to HCOOH. The Faradaic efficiency of HCOOH could be as high as 94.1% with a current density of 28.4 mA cm-2 in ionic liquid-MeCN system. The reaction mechanism was proposed on the basis of some control experiments. This work opens a new way to prepare composite electrode for electrochemical reduction of CO_2.展开更多
Electroreduction of carbon dioxide(CO_(2))to value-added chemicals and fuels is a promising approach for sustainable energy conversion and storage.Many electrocatalysts have been designed for this purpose and studied ...Electroreduction of carbon dioxide(CO_(2))to value-added chemicals and fuels is a promising approach for sustainable energy conversion and storage.Many electrocatalysts have been designed for this purpose and studied extensively.The role of the electrolyte is particularly interesting and is pivotal for designing electrochemical devices by taking advantage of the synergy between electrolyte and catalyst.Recently,ionic liquids as electrolytes have received much attention due to their high CO2 adsorption capacity,high selectivity,and low energy consumption.展开更多
文摘The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject.Cu-based bimetallic catalysts are extremely promising for efficient CO2 reduction.In this work,we synthesize a series of porous bimetallic Cu–Sb alloys with different compositions for the catalytic reduction of CO2 to C2H4.It is demonstrated that the alloy catalysts are much more efficient than the pure Cu catalyst.The performance of the alloy catalysts depended strongly on the composition.Further,the alloy with a Cu:Sb ratio of 10:1 yielded the best results;it exhibited a high C2H4 Faradaic efficiency of 49.7%and a high current density of 28.5 mA cm?2 at?1.19 V vs.a reversible hydrogen electrode(RHE)in 0.1 M KCl solution.To the best of our knowledge,the electrocatalytic reduction of CO2 to C2H4 using Cu–Sb alloys as catalysts has not been reported.The excellent performance of the porous alloy catalyst is attributed to its favorable electronic configuration,large surface area,high CO2 adsorption rate,and fast charge transfer rate.
基金the National Natural Science Foundation of China(grant nos.22073104,22273108,22293015,22072156,and 22121002)the Beijing Natural Science Foundation(grant no.2222043)+1 种基金the CAS Project for Young Scientists in Basic Research(grant no.YSBR-050)the Innovation Program of the IHEP(grant no.2023000034)for their financial support of this research。
文摘The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is critical.Here,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the electroreduction of related metallic oxides in quaternary ammonium surfactant solutions.Compared to their physical adsorption,cations embedded into the electrodes have a more pronounced impact on the electrical field,which effectively influences the adsorption state of intermediates.With the increase of surface field,the hydrogen evolution reaction and*COOH route are significantly reduced,favouring the*OCHO pathway instead.As a result,hydrogen,CO,and C_(2+)products almost completely vanish at−0.5 V versus RHE in 0.1 M Na_(2)SO_(4)in an H-type cell after enough cations are embedded into the Cu electrode,and the faradaic efficiency of formate rises from 18.0%to 99.5%simultaneously.
基金supported by the National Natural Science Foundation of China (21403253, 21533011)
文摘Electrochemical reduction of CO_2 to CO is an interesting topic. In this work, we prepared metal-free electrodes by depositing graphene oxide(GO), multi-walled carbon nanotube(MWCNT), and GO/MWCNT composites on carbon paper(CP) using electrophoretic deposition(EPD) method. The electrodes were characterized by different methods, such as X-ray diffraction(XRD) and X-ray photoelectron spectroscopy(XPS). The electrochemical reduction of CO_2 to CO was conducted on the electrodes in 1-butyl-3-methylimidazolium tetrafluoroborate([Bmim]BF4)/acetonitrile(Me CN) electrolyte, and the composition of the electrolyte influenced the reaction significantly. It was demonstrated that GO/MWCNT-CP electrode was very effective for the reaction in IL(90 wt%)/Me CN binary mixture, the Faradaic efficiency of CO and current density were even higher than those on Au and Ag electrodes in the same electrolyte.
基金the National Natural Science Foundation of China(22022307,22279146,22102192,22033009,21890761,22121002)CAS Project for Young Scientists in Basic Research(Grant No.YSBR-050)+2 种基金the National Key Research and Development Program of China(2020YFA0710203)Photon Science Center for Carbon Neutrality,and China Postdoctoral Science Foundation(BX20200336 and 2020M680680)In situ X-ray adsorption spectroscopy was conducted at 1W2B beamline station of Beijing Synchrotron Radiation Facility.
文摘Copper(Cu)is recognized as one of the most efficient metal catalysts that can perform the electrocatalytic CO_(2) reduction reaction(CO_(2)RR)and its surface oxidation state determines the reaction pathway.The Cuδ+(0<δ<1)species,are well known active sites in CO_(2)RR to produce hydrocarbons and oxygenates.However,Cuδ+active sites are difficult to control,and it is very easy to be reduced to Cu^(0) under CO_(2)RR operating conditions.Herein,we report a homo-hetero doping strategy to construct an efficient samarium(Sm)and sulfur(S)co-doping catalyst(Smx-CuSy)for CO_(2)RR to formic acid(HCOOH).At optimum conditions,Smx-CuSy delivered a high HCOOH Faradaic efficiency(FE)of 92.1%at the current density of 300 mA·cm^(–2) using 1 mol/L KOH aqueous solution as electrolyte,and the reduction potential was as low as–0.52 V vs.reversible hydrogen electrode(RHE).The co-doping of Sm and S resulted in excellent CO_(2)RR performance owing to the synergistic effect of the homo-hetero structure.The homo-doping of S could effectively adjust the electronic structure of Cu in favor of the formation of abundant Cu^(δ+)species.The existence of hetero-Sm species could not only stabilize the Cu^(δ+)sites,but also increase the concentration of H ions to form a favorable catalytic environment for HCOOH generation.
基金supported by the National Natural Science Foundation of China(22273108,22073104,22293015,22033009,21890761,22121002,and 12275300)Beijing Natural Science Foundation(2222043)+1 种基金Chinese Academy of Sciences(CAS)Project for Young Scientists in Basic Research(YSBR-050)the Innovation Program of the Institute of High Energy Physics,CAS(2023000034)。
基金supported by the National Natural Science Foundation of China (21673248, 21533011)the National Key Research and Development Program of China (2017YFA0403102)Chinese Academy of Sciences (QYZDY-SSW-SLH013)
文摘Electrocatalytic reduction of CO_2 is a promising route for energy storage and utilization. Herein we synthesized SnO_2 nanosheets and supported them on N-doped porous carbon (N-PC) by electrodeposition for the first time. The SnO_2 and N-PC in the SnO_2@N-PC composites had exellent synergistic effect for electrocatalytic reduction of CO_2 to HCOOH. The Faradaic efficiency of HCOOH could be as high as 94.1% with a current density of 28.4 mA cm-2 in ionic liquid-MeCN system. The reaction mechanism was proposed on the basis of some control experiments. This work opens a new way to prepare composite electrode for electrochemical reduction of CO_2.
基金The work was supported financially by the National Key Research and Development Program of China(2017YFA0403102)National Natural Science Foundation of China(21773267,21890761,21533011)the Chinese Academy of Sciences(QYZDY-SSW-SLH013).
文摘Electroreduction of carbon dioxide(CO_(2))to value-added chemicals and fuels is a promising approach for sustainable energy conversion and storage.Many electrocatalysts have been designed for this purpose and studied extensively.The role of the electrolyte is particularly interesting and is pivotal for designing electrochemical devices by taking advantage of the synergy between electrolyte and catalyst.Recently,ionic liquids as electrolytes have received much attention due to their high CO2 adsorption capacity,high selectivity,and low energy consumption.
