La0.9Sr0.1Ga0.8Mg0.2Ox固体电解质材料敏感电学特性的研究

doi:10.3724/SP.J.1077.2013.12281

无机材料学报 ›› 2013, Vol. 28 ›› Issue (4): 409-414.DOI: 10.3724/SP.J.1077.2013.12281 CSTR: 32189.14.SP.J.1077.2013.12281

La_0.9Sr_0.1Ga_0.8Mg_0.2O_x固体电解质材料敏感电学特性的研究

顾媛媛, 陈康, 江浩, 简家文

(宁波大学信息科学与工程学院, 宁波315211)

收稿日期:2012-05-02 修回日期:2012-08-19 出版日期:2013-04-10 网络出版日期:2013-03-20
作者简介:顾媛媛(1987–), 女, 硕士研究生. E-mail: 470379105@qq.com
基金资助:
国家自然科学基金(60971047);中国博士后科学基金(20100470735、2010-2012)

Research on the Sensitive Electric Properties of La_0.9Sr_0.1Ga_0.8Mg_0.2O_x Electrolyte

GU Yuan-Yuan, CHEN Kang, JIANG Hao, JIAN Jia-Wen

(Department of Information Science & Engineering, Ningbo University, Ningbo 315211, China)

Received:2012-05-02 Revised:2012-08-19 Published:2013-04-10 Online:2013-03-20
About author:GU Yuan-Yuan. E-mail: 470379105@qq.com
Supported by:
National Natural Science Foundation of China (60971047);China Postdoctoral Science Foundation (20100470735, 2010-2012)

摘要/Abstract

摘要：

La_0.9Sr_0.1Ga_0.8Mg_0.2O_x(LSGM)粉体在1000~1500℃烧结4 h得到不同LSGM样品, 对各样品进行了各项物理和电学特性测试。结果表明, 样品的线收缩率和相对密度随烧结温度的升高而增加, 1500℃烧结4 h的样品达到最大的线收缩率和相对密度, 分别为24.8%和97%。1250~1500℃烧结4 h样品物相单一, 结晶良好, 1000℃烧结4 h的样品则存在较多杂相。各样品的电导率随测试温度升高而增大, 1400℃烧结4 h的样品在各测试温度下都具有最大的电导率, 800℃时, 其电导率约为0.093 S/cm。在此研究基础上, 采用丝网印刷技术制备了基于LSGM的小孔扩散型极限电流氧传感器, 并测得其I-V特性曲线和时间响应特性。结果显示, 该传感器的I-V曲线存在较好的极限电流平台, 且极限电流和氧浓度之间存在良好的线性关系。响应和恢复时间较短, 分别为10~15 s和15~20 s, 重复性较好。

关键词: LSGM, 电导率, 固体电解质, 氧传感器

Abstract:

La_0.9Sr_0.1Ga_0.8Mg_0.2O_x (LSGM) electrolytes were prepared from La_0.9Sr_0.1Ga_0.8Mg_0.2O_xpowders sintering at 1000-1500℃ for 4 h. Both the physical and electrical properties of the LSGM samples were tested. The results show that the linear shrinkage and relative density of the samples increase with sintering temperature rising, besides, the sample sintered at 1400℃ for 4 h shows the maximum value of 24.8% and 97%, respectively. Samples sintered at 1250℃-1500℃ for 4 h have uniform phase while that sintered at 1000℃ has a large amount of impurities. The sample sintered at 1400℃ for 4 h has the largest conductivity being 0.093 S/cm at 800℃. Based on this, a limiting-current-type O₂ sensor based on LSGM was fabricated by screen-printing technique, and the I-V characteristics and response/recovery time were measured. It shows that the I-V curves have good current plateaus, and the limiting current exhibits a linear dependence on oxygen concentration. The response/recovery time are 10-15 s and 15-20 s, respectively, showing well reproducible response characteristics.

Key words: LSGM, conductivity, electrolyte, oxygen sensor

中图分类号:

TP212

顾媛媛, 陈康, 江浩, 简家文. La_0.9Sr_0.1Ga_0.8Mg_0.2O_x固体电解质材料敏感电学特性的研究[J]. 无机材料学报, 2013, 28(4): 409-414.

GU Yuan-Yuan, CHEN Kang, JIANG Hao, JIAN Jia-Wen. Research on the Sensitive Electric Properties of La_0.9Sr_0.1Ga_0.8Mg_0.2O_x Electrolyte[J]. Journal of Inorganic Materials, 2013, 28(4): 409-414.

图/表 11

图1 基于LSGM的小孔扩散型极限电流氧传感器

Fig. 1 The limiting-current-type O2 sensor based on LSGM

图2 LSGM的线收缩率和相对密度随烧结温度的变化

Fig. 2 Linear shrinkage and relative density curve of LSGM as function of sintering temperature

图3 LSGM材料的热烧结曲线

Fig. 3 Sintering curve of LSGM

图4 不同温度烧结得到的LSGM样品的XRD图谱

Fig. 4 XRD patterns of LSGM sintered at different temperatures for 4 h

图5 不同温度烧结4 h得到LSGM样品的SEM照片

Fig. 5 SEM images of LSGM sintered at different temperatures for 4 h

图6 等效电路

Fig. 6 The equivalent circuit

图7 不同温度烧结样品的电导率随测试温度的变化情况

Fig. 7 The conductivity of LSGM sintered at different temperatures for 4 h

图8 不同温度烧结样品的Arrhenius曲线图表1 拟合参数

Fig. 8 Arrhenius plots of LSGM sintered at different temperatures for 4 h

Table 1 Fitting parameters

Sintering temperature/℃	A	B	R	E_a/ (kJ·mol^-1)
1300	14.84	-11.98	0.994	99.59
1350	15.24	-12.16	0.997	101.07
1400	14.96	-10.63	0.990	88.36
1450	16.71	-12.68	0.980	105.43
1500	15.99	-11.94	0.990	99.25

图9 氧传感器在650℃, 1%~50%不同氧浓度下的敏感特性曲线((a) I-V持性曲线, (b)极限电流和氧浓度的关系)

Fig. 9 Sensing properties of the O2 sensor based on LSGM in different gas mixtures contained 1%~50% O2 concentration at 650℃

图10 氧传感器的时间响应特性曲线

Fig. 10 The response/recovery time curves of O2 sensor

参考文献 10

[1]	Nguyen T L, Kobayashi K, Honda T, et al. Preparation and evaluation of doped ceria interlayer on supported stabilized zirconia electrolyte SOFCs by wet ceramic processes. Solid State Ionics, 2004, 174(1-4): 163-174.
[2]	JIAN Jia-Wen, YANG Bang-Chao, ZHANG Yi-Kang. Aging characteristic of Pt/YSZ electrode structure. Journal of Inorganic Materials, 2004, 19(1): 93-99.
[3]	Keqin Huang, Goodenough John B. A solid oxide fuel cell based on Sr- and Mg-doped LaGaO3 electrolyte: the role of a rare-earth oxide buffer. Journal of Alloys and Compounds, 2000, 303-304(1/2): 454-464.
[4]	Ishihara T, Matsuda H, Takita Y. Doped LaGaO3 perovskite type oxide as a new oxide ionic conductor. J. Am. Chem. Soc., 1994, 116(9): 3801-3806.
[5]	Jacobson Allan J. Materials for solid oxide fuel cells. Chem. Mater., 2010, 22(3): 660-674.
[6]	Wan Jen-Hau, Yan J Q, Goodenough J B. LSGM-based solid oxide fuel cell with 1.4 W/cm2 power density and 30 day long-yerm stability. Electrochem. Soc., 2005, 152(8): A1511-A1515.
[7]	Bi Zhonghe, Matsumoto Hiroshige, Ishihara Tatsumi. Solid-state amperometric CH4 sensor using LaGaO3-based electrolyte. Solid State Ionics, 2008, 179(27-32): 1641-1644.
[8]	衣宝廉. 燃料电池——原理•技术•应用. 北京: 化学工业出版社, 2003: 448-459.
[9]	王常珍. 固体电解质和化学传感器. 北京: 冶金工业出版社, 2000: 33-38.
[10]	刘荣辉. 中温固体氧化物燃料电池材料制备及性能研究. 昆明: 昆明理工大学博士论文, 2007.

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La_0.9Sr_0.1Ga_0.8Mg_0.2O_x固体电解质材料敏感电学特性的研究

Research on the Sensitive Electric Properties of La_0.9Sr_0.1Ga_0.8Mg_0.2O_x Electrolyte

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