钙钛矿氧化物（La_（1-x）Pr_x）_（0.6）Sr_（0.4）Co_（0.8）Fe_（0.2）O_（3-δ）的微结构与氧化学扩散性能的研究
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摘要
固体氧化物燃料电池(SOFC)具有能源综合利用率高、运行无污染等突出优点,是一种极具发展前景的新型能源转换系统,将运行温度降低到中温范围(600-800℃)是当前SOFC的一个主要发展方向。
阴极材料是SOFC的重要组件。若降低SOFC的运行温度,将引起阴极的极化过电位增加、界面电阻增大。因此,研制与电解质材料匹配性良好的新型阴极材料是发展中温SOFC的前提和基础。
本文采用固相反应法合成了(La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)(x=0.2,0.4,0.6,0.8)钙钛矿氧化物系样品,用XRD,Raman光谱等分析手段研究了其物相结构,用电导驰豫法研究了(La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)系样品的氧化学扩散性能。实验结果表明:其主结构为钙钛矿结构,随着Pr含量的增加其晶胞内的CoO_6八面体发生了畸变,其结构转变为以钙钛矿结构为主的两相共存结构。(La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)系样品的电导率随氧分压的增大而增大;氧化学扩散系数D_(chen)随温度的减小、Pr含量的增加而线性下降,在高氧分压下,D_(chen),随末态氧分压的变化不大;(La_(0.8)Pr_(0.2))_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)样品的氧扩散系数最大,在600℃时达到9.41×10~(-5)cm~2·s~(-1),是比较理想的中温固体燃料电池阴极材料。
Solid oxide fuel cell was a highly promising new energy conversion system which integrated with highlighting advantages such as energy-efficient, pollution-free. The operating temperature down to medium temperature range (600-800℃) are the major development direction of current study on SOFC.
Cathode materials are the essential components of SOFC. It should cause the increasing of polarization overpotential and interfacial resistance If lowering the operating temperature of SOFC. Therefore, develop new type of cathode materials which good matching at electrolyte material was the premise and foundation of develop IT-SOFC.
In this article, perovskite oxides of (La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)(x= 0.2,0.4,0.6,0.8) samples were obtained by solid state-reaction method. The phase structure was analysed by XRD and Raman spectrum, the oxygen chemical diffusion properties was determined by electrical conductivity relaxation technique. The resultes show that dominant phase structure of LPSCF systems is perovskite structure, the octahedral CoO_6 was some distorted with increasing of content Pr, It is reflections of the presence of different secondary phase. the conductivity of (La_(1-x)Pr_x) (0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)increases with increasing of oxygen partial pressure. The(La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)samples have higher oxygen chemical diffusion coefficients, which decrease linearity with the decreasing of temperature and increasing of content Pr. The oxygen chemical diffusion coefficients D_(chen) remains fairly constant at high PO_2. The oxygen chemical diffusion coefficients was highest at x=0.2, which achieved 9.41×10~(-5)cm~2·s~(-1) at 700℃, is comparatively potential cathodes material for intermediate temperature solid oxide fuel cells.
阴极材料是SOFC的重要组件。若降低SOFC的运行温度,将引起阴极的极化过电位增加、界面电阻增大。因此,研制与电解质材料匹配性良好的新型阴极材料是发展中温SOFC的前提和基础。
本文采用固相反应法合成了(La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)(x=0.2,0.4,0.6,0.8)钙钛矿氧化物系样品,用XRD,Raman光谱等分析手段研究了其物相结构,用电导驰豫法研究了(La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)系样品的氧化学扩散性能。实验结果表明:其主结构为钙钛矿结构,随着Pr含量的增加其晶胞内的CoO_6八面体发生了畸变,其结构转变为以钙钛矿结构为主的两相共存结构。(La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)系样品的电导率随氧分压的增大而增大;氧化学扩散系数D_(chen)随温度的减小、Pr含量的增加而线性下降,在高氧分压下,D_(chen),随末态氧分压的变化不大;(La_(0.8)Pr_(0.2))_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)样品的氧扩散系数最大,在600℃时达到9.41×10~(-5)cm~2·s~(-1),是比较理想的中温固体燃料电池阴极材料。
Solid oxide fuel cell was a highly promising new energy conversion system which integrated with highlighting advantages such as energy-efficient, pollution-free. The operating temperature down to medium temperature range (600-800℃) are the major development direction of current study on SOFC.
Cathode materials are the essential components of SOFC. It should cause the increasing of polarization overpotential and interfacial resistance If lowering the operating temperature of SOFC. Therefore, develop new type of cathode materials which good matching at electrolyte material was the premise and foundation of develop IT-SOFC.
In this article, perovskite oxides of (La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)(x= 0.2,0.4,0.6,0.8) samples were obtained by solid state-reaction method. The phase structure was analysed by XRD and Raman spectrum, the oxygen chemical diffusion properties was determined by electrical conductivity relaxation technique. The resultes show that dominant phase structure of LPSCF systems is perovskite structure, the octahedral CoO_6 was some distorted with increasing of content Pr, It is reflections of the presence of different secondary phase. the conductivity of (La_(1-x)Pr_x) (0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)increases with increasing of oxygen partial pressure. The(La_(1-x)Pr_x)_(0.6)Sr_(0.4)Co_(0.8)Fe_(0.2)O_(3-δ)samples have higher oxygen chemical diffusion coefficients, which decrease linearity with the decreasing of temperature and increasing of content Pr. The oxygen chemical diffusion coefficients D_(chen) remains fairly constant at high PO_2. The oxygen chemical diffusion coefficients was highest at x=0.2, which achieved 9.41×10~(-5)cm~2·s~(-1) at 700℃, is comparatively potential cathodes material for intermediate temperature solid oxide fuel cells.
引文
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[2]黄喜强,固体氧化物燃料电池复合电极材料的制备及性能研究,博士后工作报告,2003,4-9
[3]吕喆,固体氧化物燃料电池的理论、工艺与相关材料及其应用的研究,《哈尔滨:哈尔滨工业大学博士后研究工作报告》,2002,1-6
[4]李瑛,王林山,燃料电池[M],冶金工业出版社,2000,122-132
[5]江义,李文钊,王世忠.高温固体氧化物燃料电池进展[J],化学进展,1997,9(4),388-396
[6]吕喆,固体氧化物燃料电池的若干材料与技术问题研究(吉林大学博士学位论文),1999,1-9
[7]苏国萍.质子交换膜燃料电池内传质过程的数值模拟(硕士学位论文),山东大学,2005
[8]隋智通,隋升,罗冬梅.燃料电池及其应用[M],冶金工业出版社,2004,27-35
[9]高培德,燃料电池新进展,科技导报[J],2000(6),57-64。
[10]Jijun Xu, Research and Development on Fuel Cells-Challenges and Opportunities.Report in HUST(inter document),2002,7.
[11]姚思童,司秀丽,杨军等,燃料电池的工作原理及其发展现状,沈阳工业大学学报,1998,20(1),42-44.
[12]魏波,单气室固体氧化物燃料电池阴极材料性能的研究,哈尔滨工业大学硕士论文,2005,18-19
[13]李艳,固体氧化物燃料电池复合阴极的制备及性能研究,哈尔滨工业大学硕士论文,2004,4-6
[14]韩敏芳,彭苏萍,固体氧化物燃料电池材料及制备,科学出版社,2004,11-17
[15]魏秋明,朱时珍,高温固体氧化物燃料电池[J],中国稀土学报,1994,12(2),72-175.
[16]j.j伯顿,R.L.加坦,新型催化材料,石油工业出版社,1990,120-122
[17]L. Kindermann, D. Das, H.Nickel, etc., Chemical compatibility of the LaFeO_3 based perovskites (La_(0.4)Sr_(0.4))_zFe_(0.8)M_(0.2)O_3 (z=0.9,0.95;M=Cr,Mn,Co,Ni) with yttria stabilized zirconia[j], Solid State Ionics, 1996, 89, 215-220
[18] T.Z.Ding, Y.M.Wang, S.H.Shi, etc., Electrical transport behavior of perovskite-type oxide LSCOJ], Materials Science Letters, 2003,22(1), 1-5.
[19] H.Y.Tu, M.B.Phillipps, Y.Takeda etc., Gd_(1-x)A_xMn_(1-y)-Co[WTBZ]O_(3-δ) (A=Sr,Ca)as a cathode for solid-oxide fuel cells[J], J.Electro chem..Soc,1999,146(6),2085-2091
[20] R. Doshi, L. Richards, J.D. Carter, et al, Development of solide state fuel cells that operate at 500℃[J], J . Electrochem.Soc, 1999,146(4), 1273-1278
[21] S. P. Jian, Issues or. development of (La,Sr)MnO_3 cathode for solide oxide fuel cells[J], J. Power Sources, 2003,124(3),390-402
[22] 罗丹,骆仲泱,余春江等,中温固体氧化物燃料电池阴极La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_3的制备及其结构性能分析[J],动力工程,2006,26(6),899-903
[23] Jaroslav Cihlar, David Delfavero, Jr. et al, Syntesis, structure and oxygen thermally programmed desorption spectra of La_(1-x)Ca_xAl_(1-y)Fe_yO_3 perovskites[J], Journal of the European Ceramic Society, In Press, Corrected Proof,Available online 10 March 2006.
[24] L. W. Tai, M. M. Nasrallah, H.U. Anderson, et al, Structure and electrical properties of La_(1-x)Sr_xCo_(1-y)Fe_yO_3[J], Solide State Ionics, 1995, 76,259-271
[25] T.Ishihara,M.Honda,T.Shibayama,et al, Intermediate temperature solid oxide fuel cells using a new LaGaO_3 based oxide ion conductor[J], J.Electrochem.Soc,1998,145,3177-3183
[26] C. R. Xia, R. William, F. Chen, M. Liu, Sm_(0.5)Sr_(0.5)CoO_3 Cathodes for Low -temperature SOFCs, Solid State Ionics[J],2002,149,11-19
[27] Z.Shao,S.Haile, A High-Performance Cathode for the Next Generation of solid oxide fuel cells[J], Nature,2004,431,170-173
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