采用溶胶-凝胶法制备Sr Ti_(0.6)Fe_(0.4)O_(3-δ),通过掺杂少量YSZ制备YSZ-Sr Ti_(0.6)Fe_(0.4)O_(3-δ)复相陶瓷。采用电化学工作站测试样品电子-离子混合传导及离子传导的阻抗谱和频谱特性,结果表明,YSZ-Sr Ti_(0.6)Fe_(0.4)O_(3-δ...采用溶胶-凝胶法制备Sr Ti_(0.6)Fe_(0.4)O_(3-δ),通过掺杂少量YSZ制备YSZ-Sr Ti_(0.6)Fe_(0.4)O_(3-δ)复相陶瓷。采用电化学工作站测试样品电子-离子混合传导及离子传导的阻抗谱和频谱特性,结果表明,YSZ-Sr Ti_(0.6)Fe_(0.4)O_(3-δ)在电子-离子混合传导过程中存在三种不同的极化过程,分别来自于晶粒,晶界和电极/样品,通过等效电路对阻抗谱的拟合,活化能分别为0.16 e V,0.62 e V和0.42 e V,随温度的升高,晶粒弛豫不明显,样品电阻主要由晶界的极化过程控制;在离子传导过程中,只存在一个晶界弛豫过程,晶界弛豫随温度的升高而减小,试样的弛豫时间为~0.13-0.29 s。展开更多
采用柠檬酸-硝酸盐自蔓延燃烧法分别合成了Pr_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(PSCF)和Gd_(0.2)Ce_(0.8)O_(2-δ)(GDC)粉体,高温固相法合成La_(0.9)Sr_(0.1)Ga_(0.8)Mg_(0.2)O_(3-δ)(LSGM)电解质粉体。以LSGM为电解质,PSCF同时...采用柠檬酸-硝酸盐自蔓延燃烧法分别合成了Pr_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(PSCF)和Gd_(0.2)Ce_(0.8)O_(2-δ)(GDC)粉体,高温固相法合成La_(0.9)Sr_(0.1)Ga_(0.8)Mg_(0.2)O_(3-δ)(LSGM)电解质粉体。以LSGM为电解质,PSCF同时作为阴极和阳极,GDC作为功能层材料,构建了对称固体氧化物燃料电池PSCF│GDC│LSGM│GDC│PSCF。利用X射线衍射法研究材料的成相以及相互间的化学稳定性,交流阻抗法记录界面极化行为,用扫描电子显微镜观察电池的断面微结构,用自组装的测试系统评价电池输出性能。结果表明,合成的PSCF粉体呈立方钙钛矿结构,具有良好的氧化–还原可逆性。使用GDC功能层明显改善了氢气环境下PSCF与LSGM材料间的化学相容性以及电池的输出性能,800℃时,电极│电解质界面极化电阻从6.892?·cm^2下降到0.314?·cm^2;以加湿H_2(含体积分数3%的水蒸气)为燃料气,空气为氧化气时,单电池输出功率密度由269 m W/cm2增大至463 m W/cm^2。研究结果显示,PSCF是对称固体氧化物燃料电池良好的候选电极材料,GDC功能层对改善电池长期稳定性能具有潜在的应用价值。展开更多
LaNi（0.6）Fe（0.4）O（3-δ） （LNF） powders were synthesized by the glycine-nitrate process and LNF-gadolinium-doped ceria （GDC） nanocomposite cathodes for solid oxide fuel cells （SOFCs） were fabricated by infil...LaNi（0.6）Fe（0.4）O（3-δ） （LNF） powders were synthesized by the glycine-nitrate process and LNF-gadolinium-doped ceria （GDC） nanocomposite cathodes for solid oxide fuel cells （SOFCs） were fabricated by infiltration from LNF porous backbones. Electrochemical properties and Cr-poisoning behavior of LNF-GDC cathodes were studied. Single phase perovskite LNF could be obtained at the glycine to nitrate molar ratio of 1：1. The polarization resistance of the LNF-GDC nanocomposite cathode was significantly decreased in comparison with the LNF. This phenomenon was associated with enhanced catalytic activity and enlarged triple-phase boundary （TPB） length by GDC nano particles. In addition, the nanocomposite cathode showed good Cr tolerance under open circuit condition. The LNF-GDC nanocomposite cathodes were expected for use as a potential cathode in intermediate- temperature solid oxide fuel cells （IT-SOFC）.展开更多
Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ has been successfully prepared by using citrate-EDTA complexation method at relatively low calcination temperature. The structure and thermal decomposition process of ...Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ has been successfully prepared by using citrate-EDTA complexation method at relatively low calcination temperature. The structure and thermal decomposition process of the complex precursor have been investigated by means of differential scanning calorimetry-thermal gravimetric analysis （DSC/TGA）, X-ray diffraction （XRD）, and Fourier transform infrared spectroscopic （FT-IR） measurements. The precursor decomposed completely and started to form perovskite-type oxide above 420 ℃ according to the differential scanning calorimetry （DSC） and thermal gravimetric analysis （TGA） results. Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ obtained has been confirmed from the XRD pattern, and no peak of SrCO3 was found by XRD of the oxides synthesized at a relatively low temperature of 800℃. The reducibility of La0.6Sr0.4Co0.8Fe0.2O3-δ was also characterized by the temperature programmed reduction （TPR） technique. Disk shaped dense La0.6Sr0.4Co0.8Fe0.2O3-δ membrane was prepared by the isostatical pressing method. The oxygen flux rate of dense La0.6Sr0.4Co0.8Fe0.2O3-δ membrane was （2.8-18）× 10^-8 mol/（cm^2.s） in the temperature range of 800-1000 ℃.展开更多
文章采用柠檬酸络合法制备了La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)钙钛矿,采用低温N_2物理吸附、X-射线衍射(X-ray diffraction,XRD)、氢气程序升温还原(hydrogen temperature programmed reduction,H_2-TPR)、氧气程序升温脱附(ox...文章采用柠檬酸络合法制备了La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)钙钛矿,采用低温N_2物理吸附、X-射线衍射(X-ray diffraction,XRD)、氢气程序升温还原(hydrogen temperature programmed reduction,H_2-TPR)、氧气程序升温脱附(oxygen temperature programmed desorption,O_2-TPD)和X-射线光电子能谱(X-ray photoelectron spectroscopy,XPS)表征了其物理化学性质,并考察了甲烷催化燃烧活性。结果表明,当柠檬酸/金属离子摩尔比(citric acid to metal ions molar ratio,CMMR)为1.25时,所制得的催化剂催化活性最佳。XRD表征结果表明,CMMR为1.25或1.50时,形成的钙钛矿晶型更完整。H_2-TPR表征结果表明,CMMR为1.25时,催化剂中的Fe^(4+)和Co^(3+)的还原温度较低,还原性能好。XPS表征结果表明,CMMR为1.25时,催化剂表面上吸附氧晶格氧之比最大。O_2-TPD表征结果表明,随着CMMR增加,催化剂中可移动晶格氧量减小,脱附温度增加,非化学计量比显著减小。CMMR为1.25时,催化剂表面吸附氧较易活化,形成活性物种。展开更多
Mixed ionic-electronic conductors in the family of LaxSr1-xCoyFe1-y O3-δ have been widely studied as cathode materials for solid oxide fuel cells （SOFCs）. However, the long-term stability was a concern. Here we rep...Mixed ionic-electronic conductors in the family of LaxSr1-xCoyFe1-y O3-δ have been widely studied as cathode materials for solid oxide fuel cells （SOFCs）. However, the long-term stability was a concern. Here we report our findings on the effect of a thin film coating of La0.85Sr0.15MnO3-δ （LSM） on the performance of a porous La0.6Sr0.4Co0.2Feo.8O3-δ（LSCF） cathode. When the thicknesses of the LSM coatings are appropriate, an LSM-coated LSCF electrode showed better stability and lower polarization （or higher activity） than the blank LSCF cathode without LSM infiltration. An anode-supported cell with an LSM-infiltrated LSCF cathode demonstrated at 825 ℃ a peak power density of -1.07 W/cm2, about 24% higher than that of the same cell without LSM infiltration （-0.86 W/cm2）. Further, the LSM coating enhanced the stability of the electrode; there was little degradation in performance for the cell with an LSM-infiltrated LSCF cathode during 100 h operation.展开更多
Fluidized bed reactor is widely used in coal char-CO2 gasification. In this work, the production of syngas by using a fluidized bed gasification technique was first investigated and then the effect of the produced syn...Fluidized bed reactor is widely used in coal char-CO2 gasification. In this work, the production of syngas by using a fluidized bed gasification technique was first investigated and then the effect of the produced syngas on the performance of the solid oxide fuel cell with a configuration of La0.4Sr0.6Co0.2 Fe0.7 Nb0.1O3-δ//La0.8Sr0.2Ga0.83Mg0.17O3-δ//La0.4Sr0.6Co0.2Fe0.7Nb0.1O3-δ（LSCFN//LSGM//LSCFN） was studied. During the syngas production, we found that the volume fraction of CO increased with the increment of gasification temperature, and it reached a maximum value of 88.8%, corresponding to a composition of 0.76% H2, 88.8% CO, and 10.44% CO2, when the ratio of oxygen mass flow rate to that of coal char （Mo2/Mchar） increased to 0.29. In the following utilization of the produced syngas in solid oxide fuel cells, it was found that the increasing CO volume fraction in the syngas results in a gradual increase of the peak power density of the LSCFN//LSGM//LSCFN cell. The maximum peak power density of 410 mW/cm^2 was achieved for the syngas produced at 0.29 of Mo2/Mchar. In the stability test, the cell voltage decreased by 4% at a constant current density of 0.475 A/cm^2 after 54 h when fueled with the syngas with the composition of 0.76% H2, 88.8% CO, and 10.44% CO2. It reveals that a carbon deposition with the content of 13.66% in the anode is attributed to the cell performance degradation.展开更多
文摘采用溶胶-凝胶法制备Sr Ti_(0.6)Fe_(0.4)O_(3-δ),通过掺杂少量YSZ制备YSZ-Sr Ti_(0.6)Fe_(0.4)O_(3-δ)复相陶瓷。采用电化学工作站测试样品电子-离子混合传导及离子传导的阻抗谱和频谱特性,结果表明,YSZ-Sr Ti_(0.6)Fe_(0.4)O_(3-δ)在电子-离子混合传导过程中存在三种不同的极化过程,分别来自于晶粒,晶界和电极/样品,通过等效电路对阻抗谱的拟合,活化能分别为0.16 e V,0.62 e V和0.42 e V,随温度的升高,晶粒弛豫不明显,样品电阻主要由晶界的极化过程控制;在离子传导过程中,只存在一个晶界弛豫过程,晶界弛豫随温度的升高而减小,试样的弛豫时间为~0.13-0.29 s。
文摘采用柠檬酸-硝酸盐自蔓延燃烧法分别合成了Pr_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)(PSCF)和Gd_(0.2)Ce_(0.8)O_(2-δ)(GDC)粉体,高温固相法合成La_(0.9)Sr_(0.1)Ga_(0.8)Mg_(0.2)O_(3-δ)(LSGM)电解质粉体。以LSGM为电解质,PSCF同时作为阴极和阳极,GDC作为功能层材料,构建了对称固体氧化物燃料电池PSCF│GDC│LSGM│GDC│PSCF。利用X射线衍射法研究材料的成相以及相互间的化学稳定性,交流阻抗法记录界面极化行为,用扫描电子显微镜观察电池的断面微结构,用自组装的测试系统评价电池输出性能。结果表明,合成的PSCF粉体呈立方钙钛矿结构,具有良好的氧化–还原可逆性。使用GDC功能层明显改善了氢气环境下PSCF与LSGM材料间的化学相容性以及电池的输出性能,800℃时,电极│电解质界面极化电阻从6.892?·cm^2下降到0.314?·cm^2;以加湿H_2(含体积分数3%的水蒸气)为燃料气,空气为氧化气时,单电池输出功率密度由269 m W/cm2增大至463 m W/cm^2。研究结果显示,PSCF是对称固体氧化物燃料电池良好的候选电极材料,GDC功能层对改善电池长期稳定性能具有潜在的应用价值。
基金supported by a grant from the Fundamental R&D Program for Core Technology of Materials (No.10051006)funded by the Ministry of Knowledge Economy, Republic of Koreasupported by the New & Renewable Energy Core Technology Program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP), granted financial resource from the Ministry of Trade, Industry & Energy, Republic of Korea (No. 20113020030050)
文摘LaNi（0.6）Fe（0.4）O（3-δ） （LNF） powders were synthesized by the glycine-nitrate process and LNF-gadolinium-doped ceria （GDC） nanocomposite cathodes for solid oxide fuel cells （SOFCs） were fabricated by infiltration from LNF porous backbones. Electrochemical properties and Cr-poisoning behavior of LNF-GDC cathodes were studied. Single phase perovskite LNF could be obtained at the glycine to nitrate molar ratio of 1：1. The polarization resistance of the LNF-GDC nanocomposite cathode was significantly decreased in comparison with the LNF. This phenomenon was associated with enhanced catalytic activity and enlarged triple-phase boundary （TPB） length by GDC nano particles. In addition, the nanocomposite cathode showed good Cr tolerance under open circuit condition. The LNF-GDC nanocomposite cathodes were expected for use as a potential cathode in intermediate- temperature solid oxide fuel cells （IT-SOFC）.
基金Sponsored by SRF for ROCS, key lab of enhanced heat transfer and energy conservation (MOE)Guangdong provincial natural science foundation (04020126).
文摘Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ has been successfully prepared by using citrate-EDTA complexation method at relatively low calcination temperature. The structure and thermal decomposition process of the complex precursor have been investigated by means of differential scanning calorimetry-thermal gravimetric analysis （DSC/TGA）, X-ray diffraction （XRD）, and Fourier transform infrared spectroscopic （FT-IR） measurements. The precursor decomposed completely and started to form perovskite-type oxide above 420 ℃ according to the differential scanning calorimetry （DSC） and thermal gravimetric analysis （TGA） results. Single-phase perovskite La0.6Sr0.4Co0.8Fe0.2O3-δ obtained has been confirmed from the XRD pattern, and no peak of SrCO3 was found by XRD of the oxides synthesized at a relatively low temperature of 800℃. The reducibility of La0.6Sr0.4Co0.8Fe0.2O3-δ was also characterized by the temperature programmed reduction （TPR） technique. Disk shaped dense La0.6Sr0.4Co0.8Fe0.2O3-δ membrane was prepared by the isostatical pressing method. The oxygen flux rate of dense La0.6Sr0.4Co0.8Fe0.2O3-δ membrane was （2.8-18）× 10^-8 mol/（cm^2.s） in the temperature range of 800-1000 ℃.
文摘文章采用柠檬酸络合法制备了La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)钙钛矿,采用低温N_2物理吸附、X-射线衍射(X-ray diffraction,XRD)、氢气程序升温还原(hydrogen temperature programmed reduction,H_2-TPR)、氧气程序升温脱附(oxygen temperature programmed desorption,O_2-TPD)和X-射线光电子能谱(X-ray photoelectron spectroscopy,XPS)表征了其物理化学性质,并考察了甲烷催化燃烧活性。结果表明,当柠檬酸/金属离子摩尔比(citric acid to metal ions molar ratio,CMMR)为1.25时,所制得的催化剂催化活性最佳。XRD表征结果表明,CMMR为1.25或1.50时,形成的钙钛矿晶型更完整。H_2-TPR表征结果表明,CMMR为1.25时,催化剂中的Fe^(4+)和Co^(3+)的还原温度较低,还原性能好。XPS表征结果表明,CMMR为1.25时,催化剂表面上吸附氧晶格氧之比最大。O_2-TPD表征结果表明,随着CMMR增加,催化剂中可移动晶格氧量减小,脱附温度增加,非化学计量比显著减小。CMMR为1.25时,催化剂表面吸附氧较易活化,形成活性物种。
基金supported by the Department of Energy (National Energy Technology Laboratory) SECA Core Technology Program under Award Number DE-NT0006557 and DE-FE0009652by NSFC under grant No.51002182
文摘Mixed ionic-electronic conductors in the family of LaxSr1-xCoyFe1-y O3-δ have been widely studied as cathode materials for solid oxide fuel cells （SOFCs）. However, the long-term stability was a concern. Here we report our findings on the effect of a thin film coating of La0.85Sr0.15MnO3-δ （LSM） on the performance of a porous La0.6Sr0.4Co0.2Feo.8O3-δ（LSCF） cathode. When the thicknesses of the LSM coatings are appropriate, an LSM-coated LSCF electrode showed better stability and lower polarization （or higher activity） than the blank LSCF cathode without LSM infiltration. An anode-supported cell with an LSM-infiltrated LSCF cathode demonstrated at 825 ℃ a peak power density of -1.07 W/cm2, about 24% higher than that of the same cell without LSM infiltration （-0.86 W/cm2）. Further, the LSM coating enhanced the stability of the electrode; there was little degradation in performance for the cell with an LSM-infiltrated LSCF cathode during 100 h operation.
基金financially supported by the National Basic Research Program of China (Grant Nos. 2012CB215404, 2012CB215406)State Key Laboratory of Power Systems in Tsinghua University (No. SKLD15Z02, Fuel Cell Distributed Power Generation System)One-hundred Leading Talents Development Project for Progress on Science and Technology of Beijing (No. 041504130)
文摘Fluidized bed reactor is widely used in coal char-CO2 gasification. In this work, the production of syngas by using a fluidized bed gasification technique was first investigated and then the effect of the produced syngas on the performance of the solid oxide fuel cell with a configuration of La0.4Sr0.6Co0.2 Fe0.7 Nb0.1O3-δ//La0.8Sr0.2Ga0.83Mg0.17O3-δ//La0.4Sr0.6Co0.2Fe0.7Nb0.1O3-δ（LSCFN//LSGM//LSCFN） was studied. During the syngas production, we found that the volume fraction of CO increased with the increment of gasification temperature, and it reached a maximum value of 88.8%, corresponding to a composition of 0.76% H2, 88.8% CO, and 10.44% CO2, when the ratio of oxygen mass flow rate to that of coal char （Mo2/Mchar） increased to 0.29. In the following utilization of the produced syngas in solid oxide fuel cells, it was found that the increasing CO volume fraction in the syngas results in a gradual increase of the peak power density of the LSCFN//LSGM//LSCFN cell. The maximum peak power density of 410 mW/cm^2 was achieved for the syngas produced at 0.29 of Mo2/Mchar. In the stability test, the cell voltage decreased by 4% at a constant current density of 0.475 A/cm^2 after 54 h when fueled with the syngas with the composition of 0.76% H2, 88.8% CO, and 10.44% CO2. It reveals that a carbon deposition with the content of 13.66% in the anode is attributed to the cell performance degradation.
