Solid oxide electrolysis cell(SOEC) can electrochemically convert CO2 to CO at the gas-solid interface with a high current density and Faradaic efficiency, which has attracted increasing attentions in recent years.Exp...Solid oxide electrolysis cell(SOEC) can electrochemically convert CO2 to CO at the gas-solid interface with a high current density and Faradaic efficiency, which has attracted increasing attentions in recent years.Exploring efficient catalyst for electrochemical CO2 reduction reaction(CO2 RR) at the cathode is a grand challenge for the research and development of SOEC. Sr2Fe1.5Mo0.5O6-δ(SFM) is one kind of promising cathode materials for SOEC, but suffers from insufficient activity for CO2 RR. Herein, Gd0.2Ce0.8O1.9(GDC)nanoparticles were infiltrated onto the SFM surface to construct a composite GDC-SFM cathode and improve the CO2 RR performance in SOEC. The current density over the GDC infiltrated SFM cathode with a GDC loading of 12.8 wt% reaches 0.446 A cm-2 at 1.6 V and 800 °C, which is much higher than that over the SFM cathode(0.283 A cm-2). Temperature-programmed desorption of CO2 measurements suggest that the infiltration of GDC nanoparticles significantly increases the density of surface active sites and three phase boundaries(TPBs), which are beneficial for CO2 adsorption and subsequent conversion. Electrochemical impedance spectroscopy results indicate that the polarization resistance of 12.8 wt% GDCSFM cathode was obviously decreased from 0.46 to 0.30 cm^2 after the infiltration of GDC nanoparticles.展开更多
Gold, as the common current collector in solid oxide electrolysis cell(SOEC), is traditionally considered to be inert for oxygen evolution reaction at the anode of SOEC. Herein, gold nanoparticles were loaded onto con...Gold, as the common current collector in solid oxide electrolysis cell(SOEC), is traditionally considered to be inert for oxygen evolution reaction at the anode of SOEC. Herein, gold nanoparticles were loaded onto conventional strontium doped lanthanum manganite-yttria stabilized zirconia(LSM-YSZ) anode, which evidently improved the performance of oxygen evolution reaction at 800 °C. The current densities at 1.2 V and 1.4 V increased by 60.0% and 46.9%, respectively, after loading gold nanoparticles onto the LSM-YSZ anode. Physicochemical characterizations and electrochemical measurements suggested that the improved SOEC performance was attributed to the accelerated electron transfer of elementary process in anodic polarization reaction and the newly generated triple phase boundaries in gold nanoparticles-loaded LSMYSZ anode.展开更多
Feasible construction of cathode materials with highly dispersed active sites can extend the tri‐ple‐phase boundaries,and therefore leading to enhanced electrode kinetics for CO_(2) electrolysis in solid oxide elect...Feasible construction of cathode materials with highly dispersed active sites can extend the tri‐ple‐phase boundaries,and therefore leading to enhanced electrode kinetics for CO_(2) electrolysis in solid oxide electrolysis cell(SOEC).Herein,highly dispersed nickel species with low loading(1.0 wt%)were trapped within the La_(0.8)Sr_(0.2)FeO_(3)–δ‐Ce_(0.8)Sm_(0.2)O_(2)–δvia a facial mechanical milling ap‐proach,which demonstrated excellent CO_(2) electrolysis performance.The highly dispersed nickel species can significantly alter the electronic structures of the LSF‐SDC without affecting its porous network and facilitate oxygen vacancy formation,thus greatly promote the CO_(2) electrolysis perfor‐mance.The highest current density of 1.53 A·cm^(-2) could be achieved when operated under 800℃ at 1.6 V,which is about 91%higher than the LSF‐SDC counterpart.展开更多
Solid oxide electrolysis cell(SOEC)is a promising technology for CO_(2) conversion and renewable energy storage with high efficiency.It is highly desirable to develop catalytically active cathodes for CO_(2) electroly...Solid oxide electrolysis cell(SOEC)is a promising technology for CO_(2) conversion and renewable energy storage with high efficiency.It is highly desirable to develop catalytically active cathodes for CO_(2) electrolysis.Herein,cathode materials with different structural stabilities are designed by Nb substitution on La_(0.5)Sr_(0.5)Fe_(0.8)Co_(0.2)O_(3-δ)(LSFC82)to obtain La_(0.5)Sr_(0.5)Fe_(0.7)Co_(0.2)Nb_(0.1)O_(3-δ)(LSFCN721)and La_(0.5)Sr_(0.5)Fe_(0.8)Co_(0.1)Nb_(0.1)O_(3-δ)(LSFCN811),respectively.LSFC82-Sm_(0.2)Ce_(0.8)O_(2-δ)(SDC)cathode with inferior structural stability(ability to maintain the structure)shows desirable CO_(2) electrolysis performance with the generated current density of 1.80 A cm^(-2)2 at 1.6 V and stable performance during 110 h operation at 1.2 V and 800℃.However,LSFC82 particles are collapsed into pieces after stability test with the generation of Co nanoparticles simultaneously.The frameworks of LSFCN721 and LSFCN811 particles maintain well because of the high-valent niobium,but Co exsolution,ox-ygen vacancy content and the corresponding CO_(2) electrolysis performance are restricted.This work confirms that Co nanoparticles can be exsolved from LSFC82-SDC cathode during CO_(2) electrolysis,providing references for constructing metallic nanoparticles decorated-perovskite cathodes for SOECs.展开更多
基金financial support from the Ministry of Science and Technology of China(Grant no.2017YFA0700102)the National Natural Science Foundation of China(Grants nos.21573222,91545202 and 21703237)+3 种基金Dalian Institute of Chemical Physics(Grant no.DICP DMTO201702)Dalian Outstanding Young Scientist Foundation(Grant no.2017RJ03)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant no.XDB17020200)the financial support from CAS Youth Innovation Promotion(Grant no.2015145)
文摘Solid oxide electrolysis cell(SOEC) can electrochemically convert CO2 to CO at the gas-solid interface with a high current density and Faradaic efficiency, which has attracted increasing attentions in recent years.Exploring efficient catalyst for electrochemical CO2 reduction reaction(CO2 RR) at the cathode is a grand challenge for the research and development of SOEC. Sr2Fe1.5Mo0.5O6-δ(SFM) is one kind of promising cathode materials for SOEC, but suffers from insufficient activity for CO2 RR. Herein, Gd0.2Ce0.8O1.9(GDC)nanoparticles were infiltrated onto the SFM surface to construct a composite GDC-SFM cathode and improve the CO2 RR performance in SOEC. The current density over the GDC infiltrated SFM cathode with a GDC loading of 12.8 wt% reaches 0.446 A cm-2 at 1.6 V and 800 °C, which is much higher than that over the SFM cathode(0.283 A cm-2). Temperature-programmed desorption of CO2 measurements suggest that the infiltration of GDC nanoparticles significantly increases the density of surface active sites and three phase boundaries(TPBs), which are beneficial for CO2 adsorption and subsequent conversion. Electrochemical impedance spectroscopy results indicate that the polarization resistance of 12.8 wt% GDCSFM cathode was obviously decreased from 0.46 to 0.30 cm^2 after the infiltration of GDC nanoparticles.
基金financial support from the National Key R&D Program of China (Grant 2017YFA0700102)the National Natural Science Foundation of China (Grants 21573222 and 91545202)+4 种基金Dalian National Laboratory for Clean Energy (DNL180404)Dalian Institute of Chemical Physics (Grant DICP DMTO201702)Dalian Outstanding Young Scientist Foundation (Grant 2017RJ03)the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant no. XDB17020200)the financial support from CAS Youth Innovation Promotion (Grant no. 2015145)
文摘Gold, as the common current collector in solid oxide electrolysis cell(SOEC), is traditionally considered to be inert for oxygen evolution reaction at the anode of SOEC. Herein, gold nanoparticles were loaded onto conventional strontium doped lanthanum manganite-yttria stabilized zirconia(LSM-YSZ) anode, which evidently improved the performance of oxygen evolution reaction at 800 °C. The current densities at 1.2 V and 1.4 V increased by 60.0% and 46.9%, respectively, after loading gold nanoparticles onto the LSM-YSZ anode. Physicochemical characterizations and electrochemical measurements suggested that the improved SOEC performance was attributed to the accelerated electron transfer of elementary process in anodic polarization reaction and the newly generated triple phase boundaries in gold nanoparticles-loaded LSMYSZ anode.
文摘Feasible construction of cathode materials with highly dispersed active sites can extend the tri‐ple‐phase boundaries,and therefore leading to enhanced electrode kinetics for CO_(2) electrolysis in solid oxide electrolysis cell(SOEC).Herein,highly dispersed nickel species with low loading(1.0 wt%)were trapped within the La_(0.8)Sr_(0.2)FeO_(3)–δ‐Ce_(0.8)Sm_(0.2)O_(2)–δvia a facial mechanical milling ap‐proach,which demonstrated excellent CO_(2) electrolysis performance.The highly dispersed nickel species can significantly alter the electronic structures of the LSF‐SDC without affecting its porous network and facilitate oxygen vacancy formation,thus greatly promote the CO_(2) electrolysis perfor‐mance.The highest current density of 1.53 A·cm^(-2) could be achieved when operated under 800℃ at 1.6 V,which is about 91%higher than the LSF‐SDC counterpart.
基金We gratefully acknowledge financial support from the National Key R&D Program of China(Grant 2017YFA0700102)the National Natural Science Foundation of China(Grants 92045302 and 22072146)+1 种基金the DNL Cooperation Fund,CAS(DNL201923)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant XDB17020200).
文摘Solid oxide electrolysis cell(SOEC)is a promising technology for CO_(2) conversion and renewable energy storage with high efficiency.It is highly desirable to develop catalytically active cathodes for CO_(2) electrolysis.Herein,cathode materials with different structural stabilities are designed by Nb substitution on La_(0.5)Sr_(0.5)Fe_(0.8)Co_(0.2)O_(3-δ)(LSFC82)to obtain La_(0.5)Sr_(0.5)Fe_(0.7)Co_(0.2)Nb_(0.1)O_(3-δ)(LSFCN721)and La_(0.5)Sr_(0.5)Fe_(0.8)Co_(0.1)Nb_(0.1)O_(3-δ)(LSFCN811),respectively.LSFC82-Sm_(0.2)Ce_(0.8)O_(2-δ)(SDC)cathode with inferior structural stability(ability to maintain the structure)shows desirable CO_(2) electrolysis performance with the generated current density of 1.80 A cm^(-2)2 at 1.6 V and stable performance during 110 h operation at 1.2 V and 800℃.However,LSFC82 particles are collapsed into pieces after stability test with the generation of Co nanoparticles simultaneously.The frameworks of LSFCN721 and LSFCN811 particles maintain well because of the high-valent niobium,but Co exsolution,ox-ygen vacancy content and the corresponding CO_(2) electrolysis performance are restricted.This work confirms that Co nanoparticles can be exsolved from LSFC82-SDC cathode during CO_(2) electrolysis,providing references for constructing metallic nanoparticles decorated-perovskite cathodes for SOECs.