Activities of FeO in CaO-SiO2-Al2O3-MgO-FeO slags were determined at 1673 K by electrochemical of the solid electrolyte cell: Mo [Mo+MoOu[ZrO2(MgO)[Fe+(CaO-SiO2-Al2O3-MgO-FeO)+Ag[Fe. The influences of slag com...Activities of FeO in CaO-SiO2-Al2O3-MgO-FeO slags were determined at 1673 K by electrochemical of the solid electrolyte cell: Mo [Mo+MoOu[ZrO2(MgO)[Fe+(CaO-SiO2-Al2O3-MgO-FeO)+Ag[Fe. The influences of slag compositions and basicity on FeO activities were analyzed. The results reveal that, for slags of fixed (%CaO)/(%SiO2) ratio, MgO and Al2O3 content, there was an increase of FeO activities with increase of FeO content. For slags with constant {(%CaO)+ (%MgO)}/(%SiO2) ratio, fixed FeO and A1203 content, FeO activities decreased when MgO content increased from 5% to 10%, and increased with the increase of MgO content when it was over 10%. The FeO activities increased when (%CaO)/(%SiO2) ratio changed from 1.03 to 1.30 in the slags of constant MgO, FeO and Al2O3 content.展开更多
Industrial fly ash-derived SiO2aerogel with abundant mesopores has an excellent ability to support active ingredients for constructing efficient and stable catalyst in electrochemical CO2reduction reaction(CO_(2...Industrial fly ash-derived SiO2aerogel with abundant mesopores has an excellent ability to support active ingredients for constructing efficient and stable catalyst in electrochemical CO2reduction reaction(CO2RR).However,how to select and arrange active sites on its surface poses significant challenges due to its non-conductive nature.Here,we subtly designed and synthesized multi-component architectures to achieve the high efficiency of CO2RR to CO.The embedding of active and amorphous nitrogen-doped carbon(NC)nanosheets on the surface and inside of SiO2aerogel ensures the charge transport on the catalyst surface,and Er2O3improves dissociation of H2O,enabling the supply of protons for CO2RR.Simultaneously,Er2O3-induced defects/vacancies,nanoclusters coordinated with N on amorphous NC and single Ni in NC play crucial role in enhancing adsorption and activation of CO2.Consequently,the Ni-Er2O3/NC-SiO2catalyst exhibits the maintenance of FECOhigher than 95%over a wide potential window(-0.22 to-1.12 V vs.RHE)in a flow cell with gas-liquid-solid electrode.This work not only provides an atomistic understanding of nature of active sites in CO2RR but also contributes to the secondary utilization of industrial fly ash for a carbon-neutral future.展开更多
基金Project supported by the National Natural Science Foundation of China (Grant No.50574036)
摘要Activities of FeO in CaO-SiO2-Al2O3-MgO-FeO slags were determined at 1673 K by electrochemical of the solid electrolyte cell: Mo [Mo+MoOu[ZrO2(MgO)[Fe+(CaO-SiO2-Al2O3-MgO-FeO)+Ag[Fe. The influences of slag compositions and basicity on FeO activities were analyzed. The results reveal that, for slags of fixed (%CaO)/(%SiO2) ratio, MgO and Al2O3 content, there was an increase of FeO activities with increase of FeO content. For slags with constant {(%CaO)+ (%MgO)}/(%SiO2) ratio, fixed FeO and A1203 content, FeO activities decreased when MgO content increased from 5% to 10%, and increased with the increase of MgO content when it was over 10%. The FeO activities increased when (%CaO)/(%SiO2) ratio changed from 1.03 to 1.30 in the slags of constant MgO, FeO and Al2O3 content.
基金National Natural Science Foundation of China(22468034,22162019,22261040)Key Research and Development Project of Ordos(YF20240062)Science and Technology Projects of Inner Mongolia Autonomous Region(2021GG0195)。
摘要Industrial fly ash-derived SiO2aerogel with abundant mesopores has an excellent ability to support active ingredients for constructing efficient and stable catalyst in electrochemical CO2reduction reaction(CO2RR).However,how to select and arrange active sites on its surface poses significant challenges due to its non-conductive nature.Here,we subtly designed and synthesized multi-component architectures to achieve the high efficiency of CO2RR to CO.The embedding of active and amorphous nitrogen-doped carbon(NC)nanosheets on the surface and inside of SiO2aerogel ensures the charge transport on the catalyst surface,and Er2O3improves dissociation of H2O,enabling the supply of protons for CO2RR.Simultaneously,Er2O3-induced defects/vacancies,nanoclusters coordinated with N on amorphous NC and single Ni in NC play crucial role in enhancing adsorption and activation of CO2.Consequently,the Ni-Er2O3/NC-SiO2catalyst exhibits the maintenance of FECOhigher than 95%over a wide potential window(-0.22 to-1.12 V vs.RHE)in a flow cell with gas-liquid-solid electrode.This work not only provides an atomistic understanding of nature of active sites in CO2RR but also contributes to the secondary utilization of industrial fly ash for a carbon-neutral future.