Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode ...Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode activity and stability is a tricky problem to be addressed for SOECs.Hence,it is urgent to develop suitable cathode materials with excellent catalytic activity and stability for further practical application of SOECs.Herein,a reduced perovskite oxide,Pr_(0.35)Sr_(0.6)Fe_(0.7)Cu_(0.2)Mo_(0.1)O_(3-δ)(PSFCM0.35),is developed as SOECs cathode to electrolyze CO_(2).After reduction in 10%H_(2)/Ar,Cu and Fe nanoparticles are exsolved from the PSFCM0.35 lattice,resulting in a phase transformation from cubic perovskite to Ruddlesden-Popper(RP)perovskite with more oxygen vacancies.The exsolved metal nanoparticles are tightly attached to the perovskite substrate and afford more active sites to accelerate CO_(2)adsorption and dissociation on the cathode surface.The significantly strengthened CO_(2)adsorption capacity obtained after reduction is demonstrated by in situ Fourier transform-infrared(FT-IR)spectra.Symmetric cells with the reduced PSFCM0.35(R-PSFCM0.35)electrode exhibit a low polarization resistance of 0.43Ωcm^(2)at 850℃.Single electrolysis cells with the R-PSFCM0.35 cathode display an outstanding current density of 2947 mA cm^(-2)at 850℃and 1.6 V.In addition,the catalytic stability of the R-PSFCM0.35 cathode is also proved by operating at 800℃with an applied constant current density of 600 mA cm^(-2)for 100 h.展开更多
High-temperature CO_(2)electrolysis via solid oxide electrolysis cells(CO_(2)-SOECs)has drawn special attention due to the high energy convention efficiency,fast electrode kinetics,and great potential in carbon cyclin...High-temperature CO_(2)electrolysis via solid oxide electrolysis cells(CO_(2)-SOECs)has drawn special attention due to the high energy convention efficiency,fast electrode kinetics,and great potential in carbon cycling.However,the development of cathode materials with high catalytic activity and chemical stability for pure CO_(2)electrolysis is still a great challenge.In this work,A-site cation deficient dual-phase material,namely(Pr_(0.4)Ca_(0.6))_(x)Fe_(0.8)Ni_(0.2)O_(3-δ)(PCFN,x=1,0.95,and 0.9),has been designed as the fuel electrode for a pure CO_(2)-SOEC,which presents superior electrochemical performance.Among all these compositions,(Pr_(0.4)Ca_(0.6))_(0.95)Fe_(0.8)Ni_(0.2)O_(3-δ)(PCFN95)exhibited the lowest polarization resistance of 0.458Ωcm^(2)at open-circuit voltage and 800℃.The application of PCFN95 as the cathode in a single cell yields an impressive electrolysis current density of 1.76 A cm^(-2)at 1.5 V and 800℃,which is 76%higher than that of single cells with stoichiometric Pr_(0.4)Ca_(0.6)Fe_(0.8)Ni_(0.2)O_(3-δ)(PCFN100)cathode.The effects of A-site deficiency on materials'phase structure and physicochemical properties are also systematically investigated.Such an enhancement in electrochemical performance is attributed to the promotion of effective CO_(2)adsorption,as well as the improved electrode kinetics resulting from the A-site deficiency.展开更多
Stro ntium-doped lanthanum ferrite(LSF)is a potential ceramic cathode for direct CO_(2) electrolysis in solid oxide electrolysis cells(SOECs),but its application is limited by insufficient catalytic activity and stabi...Stro ntium-doped lanthanum ferrite(LSF)is a potential ceramic cathode for direct CO_(2) electrolysis in solid oxide electrolysis cells(SOECs),but its application is limited by insufficient catalytic activity and stability in CO_(2)-containing atmospheres.Herein,a novel strategy is proposed to enhance the electrolytic performance as well as chemical stability,achieved by doping F into the O-site of the perovskite LSF.Doping F does not change the phase structure but reduces the cell volume and improves the chemical stability in a CO_(2)-rich atmosphere.Importantly,F doping favors oxygen vacancy formation,increases oxygen vacancy concentration,and enhances the CO_(2) adsorption capability.Meanwhile,doping with F greatly improves the kinetics of the CO_(2) reduction reaction.For example,kchem increases by 78%from3.49×10^(-4) cm s^(-1) to 6.24×10^(-4) cm s^(-1),and Dchem doubles from 4.68×10^(-5) cm^(2) s^(-1) to 9.45×10^(-5)cm^(2) s^(-1).Consequently,doping F significantly increases the electrochemical performance,such as reducing R_(p) by 52.2%from 0.226Ωcm^(2) to 0.108Ωcm^(2) at 800℃.As a result,the single cell with the Fcontaining cathode exhibits an extremely high current density of 2.58 A cm^(-2) at 800℃and 1.5 V,as well as excellent durability over 200 h for direct CO_(2) electrolysis in SOECs.展开更多
Solid oxide electrolysis cells(SOECs)can convert electricity to chemicals with high efficiency at ~600-900℃,and have attracted widespread attention in renewable energy conversion and storage.SOECs operate in the inve...Solid oxide electrolysis cells(SOECs)can convert electricity to chemicals with high efficiency at ~600-900℃,and have attracted widespread attention in renewable energy conversion and storage.SOECs operate in the inverse mode of solid oxide fuel cells(SOFCs)and therefore inherit most of the advantages of SOFC materials and energy conversion processes.However,the external bias that drives the electrochemical process will strongly change the chemical environments in both in the cathode and anode,therefore necessitating careful reconsideration of key materials and electrocatalysis processes.More importantly,SOECs provide a unique advantage of electrothermal catalysis,especially in converting stable low-carbon alkanes such as methane to ethylene with high selectivity.Here,we review the state-of-the-art of SOEC research progress in electrothermal catalysis and key materials and provide a future perspective.展开更多
This study deals with the optimization of best working conditions in molten melt for the production of hydrogen(H2) gas.Limited research has been carried out on how electrochemical process occurs through steam splitti...This study deals with the optimization of best working conditions in molten melt for the production of hydrogen(H2) gas.Limited research has been carried out on how electrochemical process occurs through steam splitting via molten hydroxide.54 combinations of cathode,anode,temperature and voltage have been investigated for the optimization of best working conditions with molten hydroxide for hydrogen gas production.All these electrochemical investigations were carried out at 225 to 300℃ temperature and 1.5 to 2.5 V applied voltage values.The current efficiency of 90.5,80.0 and 68.6% has been achieved using stainless steel anodic cell with nickel,stainless steel and platinum working cathode respectively.For nickel cathode,an increase in the current directly affected the hydrogen gas flow rate at cathode.It can be hypothesized from the noted results that increase in current is directly proportional to operating temperature and applied voltage.Higher values were noted when the applied voltages increased from 1.5 to 2.5 V at 300℃,the flow rate of hydrogen gas increased from 1.5 to 11.3 cm^(3) min^(-1),1.0 to 13 cm^(3) min^(-1) in case of electrolysis@stainless steel and@graphite anode respectively.It is observed that the current efficiency of stainless steel anodic cell was higher than the graphite anodic cell.Therefore,steam splitting with the help of molten salts has shown an encouraging alternate to current methodology for H2 fuel production.展开更多
A biocathode with microbial catalyst in place of a noble metal was successfully developed for hydrogen evolution in a microbial electrolysis cell （MEC）. The strategy for fast biocathode cultivation was demonstrated....A biocathode with microbial catalyst in place of a noble metal was successfully developed for hydrogen evolution in a microbial electrolysis cell （MEC）. The strategy for fast biocathode cultivation was demonstrated. An exoelectrogenic reaction was initially extended with an H2-full atmosphere to enrich Ha-utilizing bacteria in a MEC bioanode. This bioanode was then inversely polarized with an applied voltage in a half-cell to enrich the hydrogen-evolving biocathode. The electrocatalytic hydrogen evolution reaction （HER） kinetics of the biocathode MEC could be enhanced by increasing the bicarbonate buffer concentration from 0.05 mol·L-1 to 0.5 mol· L-1 and/or by decreasing the cathode potential from -0.9 V to - 1.3 V vs. a saturated calomel electrode （SCE）. Within the tested potential region in this study, the HER rate of the biocathode MEC was primarily influenced by the microbial catalytic capability. In addition, increasing bicarbonate concentration enhances the electric migration rate of proton carriers. As a consequence, more mass H＋ can be released to accelerate the biocathode-catalyzed HER rate. A hydrogen production rate of 8.44 m3. m 3. d1 with a current density of 951.6 A. m-3 was obtained using the biocathode MEC under a cathode potential of - 1.3 V vs. SCE and 0.4 mol· L-1 bicarbonate. This study provided information on the optimization of hydrogen production in biocathode MEC and expanded the practical applications thereof.展开更多
Considering the earth powered by intermittent renewable energy in the coming future,solid oxide electrolysis cell(SOEC)will play an indispensable role in efficient energy conversion and storage on demand.The thermolyt...Considering the earth powered by intermittent renewable energy in the coming future,solid oxide electrolysis cell(SOEC)will play an indispensable role in efficient energy conversion and storage on demand.The thermolytic and kinetic merits grant SOEC a bright potential to be directly integrated with electrical grid and downstream chemical synthesis process.Meanwhile,the scientific community are still endeavoring to pursue the SOEC assembled with better materials and operated at a more energy-efficient way.In this review article,at cell level,we focus on the recent development of electrolyte,cathode,anode and buffer layer materials for both steam and CO_(2)electrolysis.On the other hand,we also discuss the next generation SOEC operated with the assistant of other fuels to further reduce the energy consumption and enhance the productivity of the electrolyzer.And stack level,the sealant,interconnect and stack operation strategies are collectively covered.Finally,the challenges and future research direction in SOECs are included.展开更多
基金supported by the National Natural Science Foundation of China(No.22278203,No.22279057)the support of the Inner Mongolia major science and technology project(2021ZD0042),Development of integrated technology for CO_(2)emission reduction in electric power metallurgy industry
文摘Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode activity and stability is a tricky problem to be addressed for SOECs.Hence,it is urgent to develop suitable cathode materials with excellent catalytic activity and stability for further practical application of SOECs.Herein,a reduced perovskite oxide,Pr_(0.35)Sr_(0.6)Fe_(0.7)Cu_(0.2)Mo_(0.1)O_(3-δ)(PSFCM0.35),is developed as SOECs cathode to electrolyze CO_(2).After reduction in 10%H_(2)/Ar,Cu and Fe nanoparticles are exsolved from the PSFCM0.35 lattice,resulting in a phase transformation from cubic perovskite to Ruddlesden-Popper(RP)perovskite with more oxygen vacancies.The exsolved metal nanoparticles are tightly attached to the perovskite substrate and afford more active sites to accelerate CO_(2)adsorption and dissociation on the cathode surface.The significantly strengthened CO_(2)adsorption capacity obtained after reduction is demonstrated by in situ Fourier transform-infrared(FT-IR)spectra.Symmetric cells with the reduced PSFCM0.35(R-PSFCM0.35)electrode exhibit a low polarization resistance of 0.43Ωcm^(2)at 850℃.Single electrolysis cells with the R-PSFCM0.35 cathode display an outstanding current density of 2947 mA cm^(-2)at 850℃and 1.6 V.In addition,the catalytic stability of the R-PSFCM0.35 cathode is also proved by operating at 800℃with an applied constant current density of 600 mA cm^(-2)for 100 h.
基金supported by the U.S.Department of Energy’s Office of Energy Efficiency and Renewable Energy(EERE)under the Industrial Efficiency&Decarbonization Office award number[DE-EE0009427]the funding support by the U.S.Department of Energy(USDOE),Office of Energy Efficiency and Renewable Energy(EERE),Advanced Manufacturing Office(AMO),under DOE Idaho Operations Office under Contract No.DEAC07-05ID14517
文摘High-temperature CO_(2)electrolysis via solid oxide electrolysis cells(CO_(2)-SOECs)has drawn special attention due to the high energy convention efficiency,fast electrode kinetics,and great potential in carbon cycling.However,the development of cathode materials with high catalytic activity and chemical stability for pure CO_(2)electrolysis is still a great challenge.In this work,A-site cation deficient dual-phase material,namely(Pr_(0.4)Ca_(0.6))_(x)Fe_(0.8)Ni_(0.2)O_(3-δ)(PCFN,x=1,0.95,and 0.9),has been designed as the fuel electrode for a pure CO_(2)-SOEC,which presents superior electrochemical performance.Among all these compositions,(Pr_(0.4)Ca_(0.6))_(0.95)Fe_(0.8)Ni_(0.2)O_(3-δ)(PCFN95)exhibited the lowest polarization resistance of 0.458Ωcm^(2)at open-circuit voltage and 800℃.The application of PCFN95 as the cathode in a single cell yields an impressive electrolysis current density of 1.76 A cm^(-2)at 1.5 V and 800℃,which is 76%higher than that of single cells with stoichiometric Pr_(0.4)Ca_(0.6)Fe_(0.8)Ni_(0.2)O_(3-δ)(PCFN100)cathode.The effects of A-site deficiency on materials'phase structure and physicochemical properties are also systematically investigated.Such an enhancement in electrochemical performance is attributed to the promotion of effective CO_(2)adsorption,as well as the improved electrode kinetics resulting from the A-site deficiency.
基金supported by the National Key R&D Program of China(2021YFB4001401)the National Natural Science Foundation of China(51972298)。
文摘Stro ntium-doped lanthanum ferrite(LSF)is a potential ceramic cathode for direct CO_(2) electrolysis in solid oxide electrolysis cells(SOECs),but its application is limited by insufficient catalytic activity and stability in CO_(2)-containing atmospheres.Herein,a novel strategy is proposed to enhance the electrolytic performance as well as chemical stability,achieved by doping F into the O-site of the perovskite LSF.Doping F does not change the phase structure but reduces the cell volume and improves the chemical stability in a CO_(2)-rich atmosphere.Importantly,F doping favors oxygen vacancy formation,increases oxygen vacancy concentration,and enhances the CO_(2) adsorption capability.Meanwhile,doping with F greatly improves the kinetics of the CO_(2) reduction reaction.For example,kchem increases by 78%from3.49×10^(-4) cm s^(-1) to 6.24×10^(-4) cm s^(-1),and Dchem doubles from 4.68×10^(-5) cm^(2) s^(-1) to 9.45×10^(-5)cm^(2) s^(-1).Consequently,doping F significantly increases the electrochemical performance,such as reducing R_(p) by 52.2%from 0.226Ωcm^(2) to 0.108Ωcm^(2) at 800℃.As a result,the single cell with the Fcontaining cathode exhibits an extremely high current density of 2.58 A cm^(-2) at 800℃and 1.5 V,as well as excellent durability over 200 h for direct CO_(2) electrolysis in SOECs.
基金the National Key Research and Development Program of China(2017YFA0700102)Natural Science Foundation of China(91845202)+3 种基金Dalian National Laboratory for Clean Energy(DNL180404)Strategic Priority Research Program of Chinese Academy of Sciences(XDB2000000)Natural Science Foundation of Fujian Province(2018J01088)State Key Laboratory of Structural Chemistry(20170011,20200012)。
文摘Solid oxide electrolysis cells(SOECs)can convert electricity to chemicals with high efficiency at ~600-900℃,and have attracted widespread attention in renewable energy conversion and storage.SOECs operate in the inverse mode of solid oxide fuel cells(SOFCs)and therefore inherit most of the advantages of SOFC materials and energy conversion processes.However,the external bias that drives the electrochemical process will strongly change the chemical environments in both in the cathode and anode,therefore necessitating careful reconsideration of key materials and electrocatalysis processes.More importantly,SOECs provide a unique advantage of electrothermal catalysis,especially in converting stable low-carbon alkanes such as methane to ethylene with high selectivity.Here,we review the state-of-the-art of SOEC research progress in electrothermal catalysis and key materials and provide a future perspective.
基金the financial supports from the EPSRC (EP/J000582/1 and EP/F026412/1)Ningbo Municipal People’s Government (3315 Plan and 2014A35001-1)。
文摘This study deals with the optimization of best working conditions in molten melt for the production of hydrogen(H2) gas.Limited research has been carried out on how electrochemical process occurs through steam splitting via molten hydroxide.54 combinations of cathode,anode,temperature and voltage have been investigated for the optimization of best working conditions with molten hydroxide for hydrogen gas production.All these electrochemical investigations were carried out at 225 to 300℃ temperature and 1.5 to 2.5 V applied voltage values.The current efficiency of 90.5,80.0 and 68.6% has been achieved using stainless steel anodic cell with nickel,stainless steel and platinum working cathode respectively.For nickel cathode,an increase in the current directly affected the hydrogen gas flow rate at cathode.It can be hypothesized from the noted results that increase in current is directly proportional to operating temperature and applied voltage.Higher values were noted when the applied voltages increased from 1.5 to 2.5 V at 300℃,the flow rate of hydrogen gas increased from 1.5 to 11.3 cm^(3) min^(-1),1.0 to 13 cm^(3) min^(-1) in case of electrolysis@stainless steel and@graphite anode respectively.It is observed that the current efficiency of stainless steel anodic cell was higher than the graphite anodic cell.Therefore,steam splitting with the help of molten salts has shown an encouraging alternate to current methodology for H2 fuel production.
基金This work was financial supported by grants from the National Natural Science Foundation of China （Grant Nos. 51108014, 21373022, 21073010, 21003007 and Ul137602）, National Major Research Program （No. 2011CB935700）, Beijing Nova Program （Z1311090004 13008）, Fundamental Research Funds for the Central Universities （YWF- 10-03-021）, Research Fund for the Doctoral Program of Higher Education of China （20111102120045） and Program for New Century Excellent Talents in University.
文摘A biocathode with microbial catalyst in place of a noble metal was successfully developed for hydrogen evolution in a microbial electrolysis cell （MEC）. The strategy for fast biocathode cultivation was demonstrated. An exoelectrogenic reaction was initially extended with an H2-full atmosphere to enrich Ha-utilizing bacteria in a MEC bioanode. This bioanode was then inversely polarized with an applied voltage in a half-cell to enrich the hydrogen-evolving biocathode. The electrocatalytic hydrogen evolution reaction （HER） kinetics of the biocathode MEC could be enhanced by increasing the bicarbonate buffer concentration from 0.05 mol·L-1 to 0.5 mol· L-1 and/or by decreasing the cathode potential from -0.9 V to - 1.3 V vs. a saturated calomel electrode （SCE）. Within the tested potential region in this study, the HER rate of the biocathode MEC was primarily influenced by the microbial catalytic capability. In addition, increasing bicarbonate concentration enhances the electric migration rate of proton carriers. As a consequence, more mass H＋ can be released to accelerate the biocathode-catalyzed HER rate. A hydrogen production rate of 8.44 m3. m 3. d1 with a current density of 951.6 A. m-3 was obtained using the biocathode MEC under a cathode potential of - 1.3 V vs. SCE and 0.4 mol· L-1 bicarbonate. This study provided information on the optimization of hydrogen production in biocathode MEC and expanded the practical applications thereof.
基金supported financially by the National Key Research&Development Program of China(No.2018YFE0124700)the National Natural Science Foundation of China(Nos.22272136,22102135,22202041,22172129,52072134,U1910209,51876181 and 51972128)+2 种基金Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM)(No.HRTP-[2022]-23)and Hubei Province(Nos.2021CBA149 and 2021CFA072)the financial support from Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515010069 and 2020A1515110904)the Natural Science Foundation of Fujian Province(No.2021J01212759)。
文摘Considering the earth powered by intermittent renewable energy in the coming future,solid oxide electrolysis cell(SOEC)will play an indispensable role in efficient energy conversion and storage on demand.The thermolytic and kinetic merits grant SOEC a bright potential to be directly integrated with electrical grid and downstream chemical synthesis process.Meanwhile,the scientific community are still endeavoring to pursue the SOEC assembled with better materials and operated at a more energy-efficient way.In this review article,at cell level,we focus on the recent development of electrolyte,cathode,anode and buffer layer materials for both steam and CO_(2)electrolysis.On the other hand,we also discuss the next generation SOEC operated with the assistant of other fuels to further reduce the energy consumption and enhance the productivity of the electrolyzer.And stack level,the sealant,interconnect and stack operation strategies are collectively covered.Finally,the challenges and future research direction in SOECs are included.
