The effect of preparation routes on the physical characteristics and activity of the Ag-MnOx/C composites toward the oxygen reduction reaction (ORR) in alkaline media were studied by X-ray diffraction (XRD), X-ray...The effect of preparation routes on the physical characteristics and activity of the Ag-MnOx/C composites toward the oxygen reduction reaction (ORR) in alkaline media were studied by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), energy-dispersion spectroscopy (EDS) as well as scanning electron microscopy (SEM) and electrochemical techniques. The results show that more Ag and Mn species present on the surface of the Ag-MnOx/C composite prepared by two-step route (Ag-MnOx/C-2) compared to the one prepared by one-step route (Ag-MnOx/C-1), which contributes to its superior activity toward the ORR. The higher electron transfer number involved in the ORR can be observed on the Ag-MnOx/C-2 composite and its specific mass kinetic current at -0.6 V (vs Hg/HgO) is 46 mA/μg, which is 23 times that on the Ag/C. The peak power density of zinc-air battery with the Ag-MnOx/C-2 air electrode reaches up to 117 mW/cm^2.展开更多
Based on use of multi-dimensional models,this investigation simulates the performance of a proton exchange membrane fuel cell by varying the channel pattern.In the one-dimensional model,the porosity of the gas diffusi...Based on use of multi-dimensional models,this investigation simulates the performance of a proton exchange membrane fuel cell by varying the channel pattern.In the one-dimensional model,the porosity of the gas diffusion layer is 0.3.The model reveals the water vapor distribution of the fuel cell and demonstrates that the amount of water vapor increases linearly with the reduction reaction adjacent to the gas channel and the gas diffusion layer.Secondly,four novel tapered gas channels are simulated by a two-dimensional model.The model considers the distributions of oxygen,the pressure drop,the amount of water vapor distribution and the polarization curves.The results indicate that as the channel depth decreases,the oxygen in the tapered gas channel can be accel-erated and forced into the gas diffusion layer to improve the cell performance.The three-dimensional model is employed to simulate the phenomenon associated with four novel tapered gas channels.The results also show that the best performance is realized in the least tapered gas channel.Finally,an experimentally determined mechanism is found to be consistent with the results of the simulation.展开更多
The perovskite-type-oxide solid solution Ba0.97Ce0.8Ho0.2O3-α was prepared by high temperature solidstate reaction and its single-phase character was confirmed by X-ray diffraction. The ionic conduction of the sample...The perovskite-type-oxide solid solution Ba0.97Ce0.8Ho0.2O3-α was prepared by high temperature solidstate reaction and its single-phase character was confirmed by X-ray diffraction. The ionic conduction of the sample was investigated using electrical methods at elevated temperatures, and the performance of the hydrogen-air fuel cell using the sample as solid electrolyte was measured, which were compared with those of BaCe0.8Ho0.2O3-α. In wet hydrogen, BaCe0.8Ho0.2O3-α almost exhibits pure protonic conduction at 600-1000℃, and its protonic transport number is 1 at 600-900 ℃ and 0.99 at 1000 ℃. Similarly, Ba0.97Ce9.8Ho0.2O3-α exhibits pure protonic conduction with the protonic transport number of 1 at 600- 700℃, but its protonic conduction is slightly lower than that of BaCe0.8Ho0.2O3-α, and the protonic transport number are 0.99-0.96 at 800-1000 ℃. In wet air, the two samples both show low protonic and oxide ionic conduction. For Ba0.97Ce0.8Ho0.2O3-α, the protonic and oxide ionic transport numbers are 0.01-0.11 and 0.30-0.31 respectively, and for BaCe0.8Ho0.2O3-α, 0.01-0.09 and 0.27-0.33 respectively. Ionic conductivities of Ba0.97Ce0.8Ho0.2O3-α are higher than those of BaCe0.8Ho0.2O3-α under wet hydrogen and wet air. The performance of the fuel cell using Ba0.97Ce0.8Ho0.2O3-α as solid electrolyte is better than that of BaCe0.8Ho0.2O3-α. At 1000 ℃, its maximum short-circuit current density and power output density are 465 mA/cm^2 and 112 mW/cm^2, respectively.展开更多
A series of transition metal nitrides(MxNy,M=Fe,Co,Ni)nanoparticle(NP)composites caged in N-doped hollow porous carbon sphere(NHPCS)were prepared by impregnation and heat treatment methods.These composites combine the...A series of transition metal nitrides(MxNy,M=Fe,Co,Ni)nanoparticle(NP)composites caged in N-doped hollow porous carbon sphere(NHPCS)were prepared by impregnation and heat treatment methods.These composites combine the high catalytic activity of nitrides and the high-efficiency mass transfer characteristics of NHPCS.The oxygen reduction reaction results indicate that Fe2N/NHPCS has the synergistic catalytic performance of higher onset potential(0.96 V),higher electron transfer number(~4)and higher limited current density(1.4 times as high as that of commercial Pt/C).In addition,this material is implemented as the air catalyst for zinc−air battery that exhibits considerable specific capacity(795.1 mA·h/g)comparable to that of Pt/C,higher durability and maximum power density(173.1 mW/cm2).展开更多
Electric bicycles powered by lead-acid batteries have developed very fast for several years in China. Because the inconvenience caused by the service performance and the inconsistency to the environmental protection p...Electric bicycles powered by lead-acid batteries have developed very fast for several years in China. Because the inconvenience caused by the service performance and the inconsistency to the environmental protection policy of the lead-acid battery, the zinc-air power battery was proposed to solve the problem in this paper. The advantage and the feasibility of developing zinc-air power batteries in China have been illustrated in the paper. And, it is represented that development of electric bicycles powered by the zinc-air power battery also can accelerate this kind of battery's development in other electric vehicles, which is favorable to economic development and environmental protection.展开更多
Metal/Air batteries are considered to be promising electricity storage devices given their compactness, environmental benignity and affordability. As a commonly available metal, aluminum has received great attention s...Metal/Air batteries are considered to be promising electricity storage devices given their compactness, environmental benignity and affordability. As a commonly available metal, aluminum has received great attention since its first use as an anode in a battery. Its high specific energy (even better volumetric energy density than lithium) makes it ideal for many primary battery applications. However, the development of A1/Air cell with alkaline electrolyte has been lagged behind mainly due to the unfavorable parasitic hydrogen generation. Herein, we designed and constructed a novel A1/H_2/Air tandem fuel cell to turn the adverse parasitic reaction into a useful process. The system consists of two anodes, namely, aluminum and hydrogen, and one common air-breathing cathode. The aluminum acts as both the anode for the A1/Air sub-cell and the source to generate hydrogen for the hydrogen/air sub-cell. The aluminum/air sub-cell has an open circuit voltage of 1.45 V and the H_2/Air sub-cell of 0.95 V. We demonstrated that the maximum power output of aluminum as a fuel was largely enhanced by 31% after incorporating the H_2/Air sub-cell with the tandem concept. In addition, a passive design was utilized in our tandem system to eliminate the dependence on auxiliary pumping sub-systems so that the whole system remained neat and eliminated the dependence of energy consuming pumps or heaters which were typically applied in micro fuel cells.展开更多
This work concerns the study of HSs (Hybrid Systems) that are made up of the integration of M-HTFC (Medium and High Temperature Fuel Cell) and MGT (Micro-Gas-Turbine). Different typologies of hybrid systems are ...This work concerns the study of HSs (Hybrid Systems) that are made up of the integration of M-HTFC (Medium and High Temperature Fuel Cell) and MGT (Micro-Gas-Turbine). Different typologies of hybrid systems are taken into account, which differ from each other in their plant layouts. The plants are considered in cogenerative arrangement. The aim of this study is to carry out an energetic analysis of the HS considered to obtain an analytical expression to depict the system operating in cogenerative arrangement. An energetic comparison among the systems analyzed based on some indexes is effected, which allows an evaluation of the plants performances in cogenerative arrangement. An energetic analysis is carried out, which is based on a "black box" depiction of the plant in which the components and the mutual interactions are highlighted. The fuel cell component of the plant is not analyzed as a black box, but each element that constitutes it, is elaborated as a subsystem.展开更多
Zinc-air battery is one of the most promising next-generation energy conversion and storage systems.Green and low-cost catalysts with high oxygen reduction reaction(ORR)catalytic activity are desired to meet the requi...Zinc-air battery is one of the most promising next-generation energy conversion and storage systems.Green and low-cost catalysts with high oxygen reduction reaction(ORR)catalytic activity are desired to meet the requirements of Zinc-air batteries.Herein,poly-active centric Co3O4-CeO2/Co-N-C(ketjenblack carbon)catalysts were prepared by a facile method.The Co3O4 and CeO2 nanoparticles are uniformly anchored on the surface of Co and N doped carbon support.The half-wave potential of Co3O4-CeO2/Co-N-C in the rotating disk electrode testing is close to that of Pt/C.The Zn-air battery using Co3O4-CeO2/Co-N-C as the cathode catalyst can provide a high specific capacity of 728 mA h g^-1 at 20 mA cm^-2 and maintain a stable discharge voltage.The remarkable catalytic performance is mainly attributed to the synergistic effect among Co3O4,CeO2 and Co-N-C,the outstanding electrical conductivity and the large surface area.Benefitting from the high catalytic activity,environmental friendliness and the facile synthesis process,Co3O4-CeO2/Co-N-C catalyst lends itself well to a great prospect in the application of metalair batteries.展开更多
Rechargeable Li-O2 batteries have attracted considerable interests because of their exceptional energy density. However, the short lifetime still remained as one of the bottle-neck obstacles for the practical applicat...Rechargeable Li-O2 batteries have attracted considerable interests because of their exceptional energy density. However, the short lifetime still remained as one of the bottle-neck obstacles for the practical application of rechargeable Li-O2 batteries. The development of efficient cathode catalyst is highly desirable to reduce the energy barrier of Li-O2 reaction and electrode failure. In this work, we report a facile strategy for the fabrication of a high-per- formance cathode catalyst for rechargeable Li-O2 batteries by the encapsulation of high content of active Fe nanorods into N-doped carbon nanotubes with high stability (denoted as Fe@NCNTs). First-principles calculations reveal that the synergistic charge transfer and redistribution between the interface of Fe nanorods, the CNT walls and the active N dopants greatly facilitate the chemisorption and subsequent dissociation of O2 molecules into the epoxy intermediates on the carbon surface, which benefits the uniform growth of nanosized discharge products on CNT surface and thus boosts the reversibility of Li-O2 reactions. As a result, the cathode with Fe@NCNT catalyst exhibRs long cycling sta- bility with high capacities (1000 mA h g-1 for 160 cycles and 600 mA h g-t for 270 cycles). Based on the total mass of Fe@NCNTs + Li2O2, high gravimetric energy densities of 2120-2600 W h kg-~ can be achieved at the power densities of 50-795 W kg-1.展开更多
Mass production of highly efficient,durable,and inexpensive single atomic catalysts is currently the major challenge associated with the oxygen reduction reaction(ORR)for fuel cells.In this study,we develop a general ...Mass production of highly efficient,durable,and inexpensive single atomic catalysts is currently the major challenge associated with the oxygen reduction reaction(ORR)for fuel cells.In this study,we develop a general strategy that uses a simple ultrasonic atomization coupling with pyrolysis and calcination process to synthesize single atomic FeNC catalysts(FeNC SACs)at large scale.The microstructure characterizations confirm that the active centers root in the single atomic Fe sites chelating to the four-fold pyridinic N atoms.The identified specific Fe active sites with the variable valence states facilitate the transfer of electrons,endowing the FeNC SACs with excellent electrochemical ORR activity.The FeNC SACs were used as cathode catalysts in a homemade Zn-air battery,giving an open-circuit voltage(OCV)of 1.43 V,which is substantially higher than that of commercial Pt/C catalysts.This study provides a simple approach to the synthesis of single atomic catalysts at large scale.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
基金Project(21406273)supported by the National Natural Science Foundation of China
文摘The effect of preparation routes on the physical characteristics and activity of the Ag-MnOx/C composites toward the oxygen reduction reaction (ORR) in alkaline media were studied by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), energy-dispersion spectroscopy (EDS) as well as scanning electron microscopy (SEM) and electrochemical techniques. The results show that more Ag and Mn species present on the surface of the Ag-MnOx/C composite prepared by two-step route (Ag-MnOx/C-2) compared to the one prepared by one-step route (Ag-MnOx/C-1), which contributes to its superior activity toward the ORR. The higher electron transfer number involved in the ORR can be observed on the Ag-MnOx/C-2 composite and its specific mass kinetic current at -0.6 V (vs Hg/HgO) is 46 mA/μg, which is 23 times that on the Ag/C. The peak power density of zinc-air battery with the Ag-MnOx/C-2 air electrode reaches up to 117 mW/cm^2.
基金Supported by the National Science Council (NSC 97-222-E-009-067)
文摘Based on use of multi-dimensional models,this investigation simulates the performance of a proton exchange membrane fuel cell by varying the channel pattern.In the one-dimensional model,the porosity of the gas diffusion layer is 0.3.The model reveals the water vapor distribution of the fuel cell and demonstrates that the amount of water vapor increases linearly with the reduction reaction adjacent to the gas channel and the gas diffusion layer.Secondly,four novel tapered gas channels are simulated by a two-dimensional model.The model considers the distributions of oxygen,the pressure drop,the amount of water vapor distribution and the polarization curves.The results indicate that as the channel depth decreases,the oxygen in the tapered gas channel can be accel-erated and forced into the gas diffusion layer to improve the cell performance.The three-dimensional model is employed to simulate the phenomenon associated with four novel tapered gas channels.The results also show that the best performance is realized in the least tapered gas channel.Finally,an experimentally determined mechanism is found to be consistent with the results of the simulation.
基金V. ACKN0WLEDGMENT This work was supported by the National Natural Science Foundation of China (No.20171034) and the Natural Science Foundation of Education Department of Jiangsu Province (No.04KJD150218).
文摘The perovskite-type-oxide solid solution Ba0.97Ce0.8Ho0.2O3-α was prepared by high temperature solidstate reaction and its single-phase character was confirmed by X-ray diffraction. The ionic conduction of the sample was investigated using electrical methods at elevated temperatures, and the performance of the hydrogen-air fuel cell using the sample as solid electrolyte was measured, which were compared with those of BaCe0.8Ho0.2O3-α. In wet hydrogen, BaCe0.8Ho0.2O3-α almost exhibits pure protonic conduction at 600-1000℃, and its protonic transport number is 1 at 600-900 ℃ and 0.99 at 1000 ℃. Similarly, Ba0.97Ce9.8Ho0.2O3-α exhibits pure protonic conduction with the protonic transport number of 1 at 600- 700℃, but its protonic conduction is slightly lower than that of BaCe0.8Ho0.2O3-α, and the protonic transport number are 0.99-0.96 at 800-1000 ℃. In wet air, the two samples both show low protonic and oxide ionic conduction. For Ba0.97Ce0.8Ho0.2O3-α, the protonic and oxide ionic transport numbers are 0.01-0.11 and 0.30-0.31 respectively, and for BaCe0.8Ho0.2O3-α, 0.01-0.09 and 0.27-0.33 respectively. Ionic conductivities of Ba0.97Ce0.8Ho0.2O3-α are higher than those of BaCe0.8Ho0.2O3-α under wet hydrogen and wet air. The performance of the fuel cell using Ba0.97Ce0.8Ho0.2O3-α as solid electrolyte is better than that of BaCe0.8Ho0.2O3-α. At 1000 ℃, its maximum short-circuit current density and power output density are 465 mA/cm^2 and 112 mW/cm^2, respectively.
基金the National Natural Science Foundation of China(Nos.51702137,51802128)the Natural Science Foundation of Jiangsu Province,China(No.BK20181013)+1 种基金the Priority Academic Program Development of Jiangsu Higher Education Institutions,China(No.18KJB430013)the Foundation of State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering,China(No.2020-KF-20).
文摘A series of transition metal nitrides(MxNy,M=Fe,Co,Ni)nanoparticle(NP)composites caged in N-doped hollow porous carbon sphere(NHPCS)were prepared by impregnation and heat treatment methods.These composites combine the high catalytic activity of nitrides and the high-efficiency mass transfer characteristics of NHPCS.The oxygen reduction reaction results indicate that Fe2N/NHPCS has the synergistic catalytic performance of higher onset potential(0.96 V),higher electron transfer number(~4)and higher limited current density(1.4 times as high as that of commercial Pt/C).In addition,this material is implemented as the air catalyst for zinc−air battery that exhibits considerable specific capacity(795.1 mA·h/g)comparable to that of Pt/C,higher durability and maximum power density(173.1 mW/cm2).
基金Anhui Exploitation Fund of Person with Ability( 2006Z029).
文摘Electric bicycles powered by lead-acid batteries have developed very fast for several years in China. Because the inconvenience caused by the service performance and the inconsistency to the environmental protection policy of the lead-acid battery, the zinc-air power battery was proposed to solve the problem in this paper. The advantage and the feasibility of developing zinc-air power batteries in China have been illustrated in the paper. And, it is represented that development of electric bicycles powered by the zinc-air power battery also can accelerate this kind of battery's development in other electric vehicles, which is favorable to economic development and environmental protection.
文摘Metal/Air batteries are considered to be promising electricity storage devices given their compactness, environmental benignity and affordability. As a commonly available metal, aluminum has received great attention since its first use as an anode in a battery. Its high specific energy (even better volumetric energy density than lithium) makes it ideal for many primary battery applications. However, the development of A1/Air cell with alkaline electrolyte has been lagged behind mainly due to the unfavorable parasitic hydrogen generation. Herein, we designed and constructed a novel A1/H_2/Air tandem fuel cell to turn the adverse parasitic reaction into a useful process. The system consists of two anodes, namely, aluminum and hydrogen, and one common air-breathing cathode. The aluminum acts as both the anode for the A1/Air sub-cell and the source to generate hydrogen for the hydrogen/air sub-cell. The aluminum/air sub-cell has an open circuit voltage of 1.45 V and the H_2/Air sub-cell of 0.95 V. We demonstrated that the maximum power output of aluminum as a fuel was largely enhanced by 31% after incorporating the H_2/Air sub-cell with the tandem concept. In addition, a passive design was utilized in our tandem system to eliminate the dependence on auxiliary pumping sub-systems so that the whole system remained neat and eliminated the dependence of energy consuming pumps or heaters which were typically applied in micro fuel cells.
文摘This work concerns the study of HSs (Hybrid Systems) that are made up of the integration of M-HTFC (Medium and High Temperature Fuel Cell) and MGT (Micro-Gas-Turbine). Different typologies of hybrid systems are taken into account, which differ from each other in their plant layouts. The plants are considered in cogenerative arrangement. The aim of this study is to carry out an energetic analysis of the HS considered to obtain an analytical expression to depict the system operating in cogenerative arrangement. An energetic comparison among the systems analyzed based on some indexes is effected, which allows an evaluation of the plants performances in cogenerative arrangement. An energetic analysis is carried out, which is based on a "black box" depiction of the plant in which the components and the mutual interactions are highlighted. The fuel cell component of the plant is not analyzed as a black box, but each element that constitutes it, is elaborated as a subsystem.
基金financial support from the Department of Science and Technology of Guangdong Province,China(2019A050510043)Shenzhen Science and Technology Innovation Commission(JCYJ20180507183818040)。
文摘Zinc-air battery is one of the most promising next-generation energy conversion and storage systems.Green and low-cost catalysts with high oxygen reduction reaction(ORR)catalytic activity are desired to meet the requirements of Zinc-air batteries.Herein,poly-active centric Co3O4-CeO2/Co-N-C(ketjenblack carbon)catalysts were prepared by a facile method.The Co3O4 and CeO2 nanoparticles are uniformly anchored on the surface of Co and N doped carbon support.The half-wave potential of Co3O4-CeO2/Co-N-C in the rotating disk electrode testing is close to that of Pt/C.The Zn-air battery using Co3O4-CeO2/Co-N-C as the cathode catalyst can provide a high specific capacity of 728 mA h g^-1 at 20 mA cm^-2 and maintain a stable discharge voltage.The remarkable catalytic performance is mainly attributed to the synergistic effect among Co3O4,CeO2 and Co-N-C,the outstanding electrical conductivity and the large surface area.Benefitting from the high catalytic activity,environmental friendliness and the facile synthesis process,Co3O4-CeO2/Co-N-C catalyst lends itself well to a great prospect in the application of metalair batteries.
基金supported by the National Natural Science Foundation of China (NSFC, 51522203)Fok Ying Tung Education Foundation (151047)+2 种基金the Recruitment Program of Global Youth Experts (2014)Xinghai Scholarship of Dalian University of Technologythe support by the Opening Project of State Key Lab of Polymer Materials Engineering, China (Sklpme2015-4-25)
文摘Rechargeable Li-O2 batteries have attracted considerable interests because of their exceptional energy density. However, the short lifetime still remained as one of the bottle-neck obstacles for the practical application of rechargeable Li-O2 batteries. The development of efficient cathode catalyst is highly desirable to reduce the energy barrier of Li-O2 reaction and electrode failure. In this work, we report a facile strategy for the fabrication of a high-per- formance cathode catalyst for rechargeable Li-O2 batteries by the encapsulation of high content of active Fe nanorods into N-doped carbon nanotubes with high stability (denoted as Fe@NCNTs). First-principles calculations reveal that the synergistic charge transfer and redistribution between the interface of Fe nanorods, the CNT walls and the active N dopants greatly facilitate the chemisorption and subsequent dissociation of O2 molecules into the epoxy intermediates on the carbon surface, which benefits the uniform growth of nanosized discharge products on CNT surface and thus boosts the reversibility of Li-O2 reactions. As a result, the cathode with Fe@NCNT catalyst exhibRs long cycling sta- bility with high capacities (1000 mA h g-1 for 160 cycles and 600 mA h g-t for 270 cycles). Based on the total mass of Fe@NCNTs + Li2O2, high gravimetric energy densities of 2120-2600 W h kg-~ can be achieved at the power densities of 50-795 W kg-1.
基金the National Natural Science Foundation of China(NSFC,51971029)the NSFC-BRICS STI Framework Program(51861145309)+4 种基金the National S&T Major Project(2018ZX10301201)the Joint Research Project of University of Science and Technology Beijing&Taipei University of Technology(TW2018007)the“1125”Zhihui Zhengzhou Talent Project of Henan Province(39080070)the Fundamental Research Funds for the Central Universities(FRF-BR-15-027A)the fund supports from the“100 talent plan”fund of Fujian province(Contract No:2017-802)。
文摘Mass production of highly efficient,durable,and inexpensive single atomic catalysts is currently the major challenge associated with the oxygen reduction reaction(ORR)for fuel cells.In this study,we develop a general strategy that uses a simple ultrasonic atomization coupling with pyrolysis and calcination process to synthesize single atomic FeNC catalysts(FeNC SACs)at large scale.The microstructure characterizations confirm that the active centers root in the single atomic Fe sites chelating to the four-fold pyridinic N atoms.The identified specific Fe active sites with the variable valence states facilitate the transfer of electrons,endowing the FeNC SACs with excellent electrochemical ORR activity.The FeNC SACs were used as cathode catalysts in a homemade Zn-air battery,giving an open-circuit voltage(OCV)of 1.43 V,which is substantially higher than that of commercial Pt/C catalysts.This study provides a simple approach to the synthesis of single atomic catalysts at large scale.
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.