We theoretically investigate the electricity storage/generation in a reversible solid oxide cell stack. The system heat is for the first time tentatively stored in a phase-change metal when the stack is operated to ge...We theoretically investigate the electricity storage/generation in a reversible solid oxide cell stack. The system heat is for the first time tentatively stored in a phase-change metal when the stack is operated to generate electricity in a fuel cell mode and then reused to store electricity in an electrolysis mode. The state of charge （H2 frication in cathode） effectively enhances the open circuit voltages （OCVs） while the system gas pressure in electrodes also increases the OCVs. On the other hand, a higher system pressure facilitates the species diffusion in electrodes that therefore accordingly improve electrode polarizations. With the aid of recycled system heat, the roundtrip efficiency reaches as high as 92% for the repeated electricity storage and generation.展开更多
In this study,we successfully synthesized double perovskite-type oxide NdBa0.5Ca0.5Co1.5Fe0.5O5+δ(NBCCF)using a conventional wet chemical method as the oxygen electrode for reversible solid oxide electrochemical cell...In this study,we successfully synthesized double perovskite-type oxide NdBa0.5Ca0.5Co1.5Fe0.5O5+δ(NBCCF)using a conventional wet chemical method as the oxygen electrode for reversible solid oxide electrochemical cells(RSOCs).The polarization resistance(Rp)of the composite electrode NBCCFGd0.1Ce0.9O2(GDC)is only 0.079Ωcm^2 at 800℃under air.The single cell based on NBCCF-GDC electrode displays a peak power density of 0.941 W/cm^2 in fuel cell mode and a low Rp value of 0.134Ωcm^2.In electrolysis cell mode,the cell displays an outstanding oxygen evolution reaction(OER)activity and shows current density as high as 0.92 A/cm^2 with 50 vol%AH(Absolute Humidity)at 800℃and applied voltage of 1.3 V.Most importantly,the cell exhibits admirable durability of 60 h both in electrolysis mode and fuel cell mode with distinguished reversibility.All these results suggest that NBCCF is a promising candidate electrode for RSOC.展开更多
Porous Sr-doped lanthanum manganite–yttria stabilized zirconia(LSM–YSZ)oxygen electrode is prepared by an infiltration process for a reversible solid oxide fuel cell(RSOFC).X-ray diffraction and SEM analysis display...Porous Sr-doped lanthanum manganite–yttria stabilized zirconia(LSM–YSZ)oxygen electrode is prepared by an infiltration process for a reversible solid oxide fuel cell(RSOFC).X-ray diffraction and SEM analysis display that perovskite phase LSM submicro particles are evenly distributed in the porous YSZ matrix.Polarization curves and electrochemical impedance spectra are conducted for the RSOFC at 800 and 850C under both SOFC and SOEC modes.At 850℃,the single cell has the maximum power density of~726 mW/cm^(2)under SOFC mode,and electrolysis voltage of 1.35 V at 1 A/cm^(2)under SOEC mode.Fuel cell/water electrolysis cycle shows the cell has good performance stability during 6 cycles,which exhibits the LSM–YSZ oxygen electrode has high electrochemical performance and good stability.The results suggest that netw ork-like LSM–YSZ electrode made by infiltration process could be a promising oxygen electrode for high temperature RSOFCs.展开更多
Reversible solid oxide cells(SOCs)are very efficient and clean for storage and regeneration of renewable electrical energy by switching between electrolysis and fuel cell modes.One of the most critical factors governi...Reversible solid oxide cells(SOCs)are very efficient and clean for storage and regeneration of renewable electrical energy by switching between electrolysis and fuel cell modes.One of the most critical factors governing the efficiency and durability of SOCs technology is the stability of the interface between oxygen electrode and electrolyte,which is conventionally formed by sintering at a high temperature of~1000–1250℃,and which suffers from delamination problem,particularly for reversibly operated SOCs.On the other hand,our recent studies have shown that the electrode/electrolyte interface can be in situ formed by a direct assembly approach under the electrochemical polarization conditions at 800℃and lower.The direct assembly approach provides opportunities for significantly simplifying the cell fabrication procedures without the doped ceria barrier layer,enabling the utilization of a variety of high-performance oxygen electrode materials on barrier layer–free yttria-stabilized zirconia(YSZ)electrolyte.Most importantly,the in situ polarization induced interface shows a promising potential as highly active and durable interface for reversible SOCs.The objective of this progress report is to take an overview of the origin and research progress of in situ fabrication of oxygen electrodes based on the direct assembly approach.The prospect of direct assembly approach in the development of effective SOCs and in the fundamental studies of electrode/electrolyte interface reactions is discussed.展开更多
To promote the electrocatalytic activity and stability of traditional(a_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LSCF)oxygen electrodes in reversible solid oxide cells(RSOCs),conventional physical mixed method was used t...To promote the electrocatalytic activity and stability of traditional(a_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LSCF)oxygen electrodes in reversible solid oxide cells(RSOCs),conventional physical mixed method was used to prepare the Pd-LSCF composite oxygen electrode.The cell with Pd-LSCF|GDC|YSZ|Ni-YSZ configuration shows perfect electrochemical performance in both solid oxide fuel cell(SOFC)mode and solid oxide electrolysis cell(SOEC)mode.In the SOFC mode,the cell achieves a power density of 1.73 W/cm^(2)at800℃higher than that of the LSCF oxygen electrode with 1.38 W/cm^(2).In the SOEC mode,the current density at 1.5 V is 1.67 A/cm^(2)at 800℃under 50 vol%steam concentration.Moreover,the reversibility and stability of the RSOCs were tested during 192 h long-term reversible operation.The degradation rate of the cell is only 2.2%/100 h and 2.5%/100 h in the SOEC and the SOFC modes,respectively.These results confirm that compositing Pd with the LSCF oxygen electrode can considerably boost the electrochemical performance of LSCF electrode in RSOCs field.展开更多
The reversible solid oxide cell(RSOC)is an attractive technology to mutually convert power and chemicals at elevated temperatures.However,its development has been hindered mainly due to the absence of a highly active ...The reversible solid oxide cell(RSOC)is an attractive technology to mutually convert power and chemicals at elevated temperatures.However,its development has been hindered mainly due to the absence of a highly active and durable fuel electrode.Here,we report a phase-transformed CoFe-Sr_(3)Fe_(1.25)Mo_(0.75)O_(7)-δ(CoFe-SFM)fuel electrode consisting of CoFe nanoparticles and Ruddlesden-Popper-layered Sr_(3)Fe_(1.25)Mo_(0.75)O_(7)-δ(SFM)from a Sr_(2)Fe_(7/6)Mo_(0.5)Co_(1/3)O_(6)-δ(SFMCo)perovskite oxide after annealing in hydrogen and apply it to reversible CO/CO_(2)conversion in RSOC.The CoFeSFM fuel electrode shows improved catalytic activity by accelerating oxygen diffusion and surface kinetics towards the CO/CO_(2)conversion as demonstrated by the distribution of relaxation time(DRT)study and equivalent circuit model fitting analysis.Furthermore,an electrolyte-supported single cell is evaluated in the 2:1 CO-CO_(2)atmosphere at 800℃,which shows a peak power density of 259 mW cm^(-2)for CO oxidation and a current density of-0.453 A cm^(-2)at 1.3 V for CO_(2)reduction,which correspond to 3.079 and3.155 m L min-1cm^(-2)for the CO and CO_(2)conversion rates,respectively.More importantly,the reversible conversion is successfully demonstrated over 20 cyclic electrolysis and fuel cell switching test modes at 1.3 and 0.6 V.This work provides a useful guideline for designing a fuel electrode through a surface/interface exsolution process for RSOC towards efficient CO-CO_(2)reversible conversion.展开更多
In this work,La_(2)NiO_(4+δ)-Ce_(0.55)La_(0.45)O_(2−δ)(denoted as LNO-xLDC)with various LDC contents(x=0,10,20,30,and 40 wt%)were prepared and evaluated as bifunctional oxygen electrodes for reversible solid oxide c...In this work,La_(2)NiO_(4+δ)-Ce_(0.55)La_(0.45)O_(2−δ)(denoted as LNO-xLDC)with various LDC contents(x=0,10,20,30,and 40 wt%)were prepared and evaluated as bifunctional oxygen electrodes for reversible solid oxide cells(RSOCs).Compared with the pure LNO,the optimum composition of LNO-30LDC exhibited the lowest polarization resistance(Rp)of 0.53 and 0.12Ω·cm^(2)in air at 650 and 750℃,respectively.The enhanced electrochemical performance of LNO-30LDC oxygen electrode was mainly attributed to the extended triple phase boundary and more oxygen ionic transfer channels.The hydrogen electrode supported single cell with LNO-30LDC oxygen electrode displayed peak power densities of 276,401,and 521 mW·cm^(−2)at 700,750,and 800℃,respectively.Moreover,the electrolysis current density of the single cell demonstrated 526.39 mA·cm^(−2) under 1.5 V at 800℃,and the corresponding hydrogen production rate was 220.03 mL·cm^(−2)·h^(−1).The encouraging results indicated that LNO-30LDC was a promising bifunctional oxygen electrode material for RSOCs.展开更多
Sr-Co containing perovskite oxides are prospective air electrode candidates for reversible solid oxide cells(RSOCs).However,their efficiencies are limited by Sr segregation and the high thermal expansion coefficient(T...Sr-Co containing perovskite oxides are prospective air electrode candidates for reversible solid oxide cells(RSOCs).However,their efficiencies are limited by Sr segregation and the high thermal expansion coefficient(TEC)of Cobased perovskites.Herein,La_(0.6)Ca_(0.4)Fe_(0.8)Ni_(0.2)O_(3-δ)(LCa FN)is tailored as an Sr-Co-free perovskite air electrode for highperformance RSOCs.Compared with La_(0.6)Sr_(0.4)Fe_(0.8)Ni_(0.2)O_(3-δ)(LSFN)and La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LSCo F),LCa FN has a high electrical conductivity (297 S cm^(-1)),TEC compatibility(11.2×10^(-6)K^(-1)) and improved chemical stability.Moreover,LCa FN has high oxygen reduction reaction(ORR)activity with a low polarization resistance(0.06Ωcm^(2)) at 800℃.A single-cell NiYSZ/YSZ/gadolinium-doped ceria(GDC)/LCa FN-GDC operated at 800℃ yields a maximum power density of 1.08 W cm^(-2) using H_(2) as fuel.In the solid oxide electrolysis cell(SOEC)mode,the cell can achieve a current density of approximately 1.2 A cm^(-2) at 1.3 V with 70% humidity at 800℃.The cell exhibits good reversibility and remains stable in continuous SOEC and solid oxide fuel cell(SOFC)modes.These findings indicate the potential application of LCa FN as an air electrode material for RSOCs.展开更多
文摘We theoretically investigate the electricity storage/generation in a reversible solid oxide cell stack. The system heat is for the first time tentatively stored in a phase-change metal when the stack is operated to generate electricity in a fuel cell mode and then reused to store electricity in an electrolysis mode. The state of charge （H2 frication in cathode） effectively enhances the open circuit voltages （OCVs） while the system gas pressure in electrodes also increases the OCVs. On the other hand, a higher system pressure facilitates the species diffusion in electrodes that therefore accordingly improve electrode polarizations. With the aid of recycled system heat, the roundtrip efficiency reaches as high as 92% for the repeated electricity storage and generation.
基金financial support from National Key Research&Development Project(2016YFE0126900)the National Natural Science Foundation of China(51672095)+2 种基金Hubei Province(2018AAA057)the EPSRC Capital for Great Technologies Grant EP/L017008/1the China Scholarship Council for funding(201806160178)。
文摘In this study,we successfully synthesized double perovskite-type oxide NdBa0.5Ca0.5Co1.5Fe0.5O5+δ(NBCCF)using a conventional wet chemical method as the oxygen electrode for reversible solid oxide electrochemical cells(RSOCs).The polarization resistance(Rp)of the composite electrode NBCCFGd0.1Ce0.9O2(GDC)is only 0.079Ωcm^2 at 800℃under air.The single cell based on NBCCF-GDC electrode displays a peak power density of 0.941 W/cm^2 in fuel cell mode and a low Rp value of 0.134Ωcm^2.In electrolysis cell mode,the cell displays an outstanding oxygen evolution reaction(OER)activity and shows current density as high as 0.92 A/cm^2 with 50 vol%AH(Absolute Humidity)at 800℃and applied voltage of 1.3 V.Most importantly,the cell exhibits admirable durability of 60 h both in electrolysis mode and fuel cell mode with distinguished reversibility.All these results suggest that NBCCF is a promising candidate electrode for RSOC.
基金This project was sponsored by financial supports from the Major State Basic Research Development Program of China(973 Program,No.2012CB215406).
文摘Porous Sr-doped lanthanum manganite–yttria stabilized zirconia(LSM–YSZ)oxygen electrode is prepared by an infiltration process for a reversible solid oxide fuel cell(RSOFC).X-ray diffraction and SEM analysis display that perovskite phase LSM submicro particles are evenly distributed in the porous YSZ matrix.Polarization curves and electrochemical impedance spectra are conducted for the RSOFC at 800 and 850C under both SOFC and SOEC modes.At 850℃,the single cell has the maximum power density of~726 mW/cm^(2)under SOFC mode,and electrolysis voltage of 1.35 V at 1 A/cm^(2)under SOEC mode.Fuel cell/water electrolysis cycle shows the cell has good performance stability during 6 cycles,which exhibits the LSM–YSZ oxygen electrode has high electrochemical performance and good stability.The results suggest that netw ork-like LSM–YSZ electrode made by infiltration process could be a promising oxygen electrode for high temperature RSOFCs.
基金The authors thank the funding support by National Natural Science Foundation of China(21875038 and 22005055)Joint Independent Innovation Fund of Tianjin University and Fuzhou University(TF2020-10)and Australian Research Council(DP180100731 and DP180100568).
文摘Reversible solid oxide cells(SOCs)are very efficient and clean for storage and regeneration of renewable electrical energy by switching between electrolysis and fuel cell modes.One of the most critical factors governing the efficiency and durability of SOCs technology is the stability of the interface between oxygen electrode and electrolyte,which is conventionally formed by sintering at a high temperature of~1000–1250℃,and which suffers from delamination problem,particularly for reversibly operated SOCs.On the other hand,our recent studies have shown that the electrode/electrolyte interface can be in situ formed by a direct assembly approach under the electrochemical polarization conditions at 800℃and lower.The direct assembly approach provides opportunities for significantly simplifying the cell fabrication procedures without the doped ceria barrier layer,enabling the utilization of a variety of high-performance oxygen electrode materials on barrier layer–free yttria-stabilized zirconia(YSZ)electrolyte.Most importantly,the in situ polarization induced interface shows a promising potential as highly active and durable interface for reversible SOCs.The objective of this progress report is to take an overview of the origin and research progress of in situ fabrication of oxygen electrodes based on the direct assembly approach.The prospect of direct assembly approach in the development of effective SOCs and in the fundamental studies of electrode/electrolyte interface reactions is discussed.
基金Project supported by the National Key Research&Development Project(2020YFB1506304)the National Natural Science Foundation of China(52172199,52072135,52002121)。
文摘To promote the electrocatalytic activity and stability of traditional(a_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LSCF)oxygen electrodes in reversible solid oxide cells(RSOCs),conventional physical mixed method was used to prepare the Pd-LSCF composite oxygen electrode.The cell with Pd-LSCF|GDC|YSZ|Ni-YSZ configuration shows perfect electrochemical performance in both solid oxide fuel cell(SOFC)mode and solid oxide electrolysis cell(SOEC)mode.In the SOFC mode,the cell achieves a power density of 1.73 W/cm^(2)at800℃higher than that of the LSCF oxygen electrode with 1.38 W/cm^(2).In the SOEC mode,the current density at 1.5 V is 1.67 A/cm^(2)at 800℃under 50 vol%steam concentration.Moreover,the reversibility and stability of the RSOCs were tested during 192 h long-term reversible operation.The degradation rate of the cell is only 2.2%/100 h and 2.5%/100 h in the SOEC and the SOFC modes,respectively.These results confirm that compositing Pd with the LSCF oxygen electrode can considerably boost the electrochemical performance of LSCF electrode in RSOCs field.
基金financially supported by the National Natural Science Foundation (52002249,51402093 and 21706162)Guangdong Basic and Applied Basic Research Foundation (2019A1515110025 and 2017A 030313289)+3 种基金the Research Grant for Scientific Platform and Project of Guangdong Provincial Education Office (2019KTSCX151)China Postdoctoral Science Foundation (2020M682872)Shenzhen Government’s Plan of Science and Technology (JCYJ201803005125247308)Technical support from the Instrumental Analysis Center of Shenzhen University (Xili Campus) is also appreciated。
文摘The reversible solid oxide cell(RSOC)is an attractive technology to mutually convert power and chemicals at elevated temperatures.However,its development has been hindered mainly due to the absence of a highly active and durable fuel electrode.Here,we report a phase-transformed CoFe-Sr_(3)Fe_(1.25)Mo_(0.75)O_(7)-δ(CoFe-SFM)fuel electrode consisting of CoFe nanoparticles and Ruddlesden-Popper-layered Sr_(3)Fe_(1.25)Mo_(0.75)O_(7)-δ(SFM)from a Sr_(2)Fe_(7/6)Mo_(0.5)Co_(1/3)O_(6)-δ(SFMCo)perovskite oxide after annealing in hydrogen and apply it to reversible CO/CO_(2)conversion in RSOC.The CoFeSFM fuel electrode shows improved catalytic activity by accelerating oxygen diffusion and surface kinetics towards the CO/CO_(2)conversion as demonstrated by the distribution of relaxation time(DRT)study and equivalent circuit model fitting analysis.Furthermore,an electrolyte-supported single cell is evaluated in the 2:1 CO-CO_(2)atmosphere at 800℃,which shows a peak power density of 259 mW cm^(-2)for CO oxidation and a current density of-0.453 A cm^(-2)at 1.3 V for CO_(2)reduction,which correspond to 3.079 and3.155 m L min-1cm^(-2)for the CO and CO_(2)conversion rates,respectively.More importantly,the reversible conversion is successfully demonstrated over 20 cyclic electrolysis and fuel cell switching test modes at 1.3 and 0.6 V.This work provides a useful guideline for designing a fuel electrode through a surface/interface exsolution process for RSOC towards efficient CO-CO_(2)reversible conversion.
基金Science and Technology Project of Jiangxi Provincial Education Department(GJJ190734)The National Natural Science Foundation of China(51962015)。
文摘In this work,La_(2)NiO_(4+δ)-Ce_(0.55)La_(0.45)O_(2−δ)(denoted as LNO-xLDC)with various LDC contents(x=0,10,20,30,and 40 wt%)were prepared and evaluated as bifunctional oxygen electrodes for reversible solid oxide cells(RSOCs).Compared with the pure LNO,the optimum composition of LNO-30LDC exhibited the lowest polarization resistance(Rp)of 0.53 and 0.12Ω·cm^(2)in air at 650 and 750℃,respectively.The enhanced electrochemical performance of LNO-30LDC oxygen electrode was mainly attributed to the extended triple phase boundary and more oxygen ionic transfer channels.The hydrogen electrode supported single cell with LNO-30LDC oxygen electrode displayed peak power densities of 276,401,and 521 mW·cm^(−2)at 700,750,and 800℃,respectively.Moreover,the electrolysis current density of the single cell demonstrated 526.39 mA·cm^(−2) under 1.5 V at 800℃,and the corresponding hydrogen production rate was 220.03 mL·cm^(−2)·h^(−1).The encouraging results indicated that LNO-30LDC was a promising bifunctional oxygen electrode material for RSOCs.
基金supported by the National Key Research&Development Program of China(2020YFB1506304,2017YFE0129300 and 2016YFE0126900)the National Natural Science Foundation of China(52072135,51672095 and U1910209)the Major Science and Technology Innovation Project of Hubei Province(2018AAA057)。
文摘Sr-Co containing perovskite oxides are prospective air electrode candidates for reversible solid oxide cells(RSOCs).However,their efficiencies are limited by Sr segregation and the high thermal expansion coefficient(TEC)of Cobased perovskites.Herein,La_(0.6)Ca_(0.4)Fe_(0.8)Ni_(0.2)O_(3-δ)(LCa FN)is tailored as an Sr-Co-free perovskite air electrode for highperformance RSOCs.Compared with La_(0.6)Sr_(0.4)Fe_(0.8)Ni_(0.2)O_(3-δ)(LSFN)and La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(LSCo F),LCa FN has a high electrical conductivity (297 S cm^(-1)),TEC compatibility(11.2×10^(-6)K^(-1)) and improved chemical stability.Moreover,LCa FN has high oxygen reduction reaction(ORR)activity with a low polarization resistance(0.06Ωcm^(2)) at 800℃.A single-cell NiYSZ/YSZ/gadolinium-doped ceria(GDC)/LCa FN-GDC operated at 800℃ yields a maximum power density of 1.08 W cm^(-2) using H_(2) as fuel.In the solid oxide electrolysis cell(SOEC)mode,the cell can achieve a current density of approximately 1.2 A cm^(-2) at 1.3 V with 70% humidity at 800℃.The cell exhibits good reversibility and remains stable in continuous SOEC and solid oxide fuel cell(SOFC)modes.These findings indicate the potential application of LCa FN as an air electrode material for RSOCs.
