MgO或Fe2O3掺杂Ce0.8Nd0.2O1.9固体电解质的结构和电性能

doi:10.3866/PKU.WHXB201203304

物理化学学报 >> 2012, Vol. 28 >> Issue (06): 1380-1386.doi: 10.3866/PKU.WHXB201203304

MgO或Fe₂O₃掺杂Ce_0.8Nd_0.2O_1.9固体电解质的结构和电性能

刘建伟¹, 周德凤¹, 杨梅¹, 罗飞¹, 孟健²

1. 长春工业大学化学与生命科学学院, 长春 130012;
2. 中国科学院长春应用化学研究所,稀土资源利用国家重点实验室, 长春 130022

收稿日期:2011-12-14 修回日期:2012-03-29 发布日期:2012-05-17
通讯作者: 周德凤 E-mail:defengzhou65@126.com
基金资助:
国家自然科学基金(20871023)和吉林省科技发展计划项目(20101549)资助

Structure and Electrical Properties of MgO or Fe₂O₃-Doped Ce_0.8Nd_0.2O_1.9 Solid Electrolytes

LIU Jian-Wei¹, ZHOU De-Feng¹, YANG Mei¹, LUO Fei¹, MENG Jian²

1. School of Chemistry and Life Science, Changchun University of Technology, Changchun 130012, P. R. China;
2. State Key Laboratory of Rare Earth Resources Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, P. R. China

Received:2011-12-14 Revised:2012-03-29 Published:2012-05-17
Contact: ZHOU De-Feng E-mail:defengzhou65@126.com
Supported by:
The project was supported by the National Natural Science Foundation of China (20871023) and Science Research Foundation of Jilin Province, China (20101549).

摘要/Abstract

摘要： 采用溶胶-凝胶法合成SiO₂含量为0.05% (w, 质量分数)的Ce_0.8Nd_0.2O_1.9 (NDC)粉体(NDCSi). 分别将0-2.0% (x, 摩尔分数)的MgO或FeO_1.5添加到NDCSi粉体中, 经10 MPa压片后于1300 °C烧结6 h. 采用X射线衍射(XRD)、拉曼(Raman)光谱和场发射扫描电子显微镜(FE-SEM)对样品进行结构表征. 采用交流(AC)阻抗谱测试样品导电性能. 结果表明: 所有样品均呈现单一立方萤石结构. MgO或Fe₂O₃掺杂于NDCSi 体系, 均可提高材料的致密度, 降低烧结温度, 提高材料的晶界电导率和总电导率. 掺杂MgO或Fe₂O₃样品的相对密度(>93%) 高于NDC 或NDCSi ( 约86%), 有效促进了样品致密化. 掺杂Fe₂O₃ 或MgO 的样品(NDCSi+0.5FeO_1.5 或NDCSi+2.0MgO)具有最高电导率, 550 °C 时总电导率分别是6.3×10^-3 或2.9×10^-3 S·cm^-1, 是NDCSi 样品总电导率(1.1×10^-3 S·cm^-1)的5.7 和2.6 倍. MgO或Fe₂O₃掺杂于NDCSi 样品对晶界电导率的影响比晶粒电导率更明显. MgO或Fe₂O₃掺杂于NDCSi均具有烧结助剂和晶界清除剂的双重作用, 但清除杂质SiO₂的机制不同.

关键词: 固体电解质, 掺钕氧化铈, 晶界清除剂, 电导率, 烧结助剂

Abstract: A precursor powder of Ce_0.8Nd_0.2O_1.9 (NDC) containing 0.05% (mass fraction) SiO₂ as an impurity (NDCSi) was doped with 0-2.0% (molar fraction) MgO or FeO_1.5 via the sol-gel method. After pressing at 10 MPa, the samples were sintered at 1300 ° C for 6 h. The structure of the pellets was characterized by X-ray diffraction (XRD), Raman spectroscopy, and field emission scanning electron microscopy (FE-SEM). The electrical conductivity of the pellets was measured using AC impedance spectroscopy. All of the samples exhibited a cubic fluorite structure. Doping with MgO or Fe₂O₃ lowered the sintering temperature, and increased the density, grain boundaries and total conductivity of NDCSi. The relative density of the samples doped with Fe₂O₃ or MgO (>93%) was higher than those of NDC or NDCSi (about 86%), suggesting these dopants are effective at promoting densification. NDCSi + 0.5FeO_1.5 and NDCSi + 2.0MgO samples exhibited the highest conductivities of 0.63 × 10^-2 and 0.29 × 10^-2 S · cm^-1, respectively, which are 5.7 and 2.6 times larger than that of NDCSi (0.11×10^-2 S·cm^-1) at 550 °C. Doping with MgO or Fe₂O₃ had a larger effect on the grain boundary conductivity of SDCSi than the bulk conductivity. These results indicate that MgO and Fe₂O₃ are effective sintering aids as well as grain boundary scavengers with different mechanisms.

Key words: Solid electrolyte, Neodymium-doped ceria, Grain boundary scavenger, Electrical conductivity, Sintering aid

刘建伟, 周德凤, 杨梅, 罗飞, 孟健. MgO或Fe₂O₃掺杂Ce_0.8Nd_0.2O_1.9固体电解质的结构和电性能[J]. 物理化学学报, 2012, 28(06), 1380-1386. doi: 10.3866/PKU.WHXB201203304

LIU Jian-Wei, ZHOU De-Feng, YANG Mei, LUO Fei, MENG Jian. Structure and Electrical Properties of MgO or Fe₂O₃-Doped Ce_0.8Nd_0.2O_1.9 Solid Electrolytes[J]. Acta Phys. -Chim. Sin. 2012, 28(06), 1380-1386. doi: 10.3866/PKU.WHXB201203304

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201203304

https://www.whxb.pku.edu.cn/CN/Y2012/V28/I06/1380

参考文献

(1) Zhang, T. S.; Du, Z. H.; Li, S.; Kong, L. B.; Song, X. C.; Lu, J.; Ma, J. Soild State Ionics 2009, 180, 1311.  doi: 10.1016/j.ssi.2009.08.004
(2) Li, B.; Liu, Y. Y.; Wei, X.; Pan, W. J. Power Sources 2010, 195, 969.  doi: 10.1016/j.jpowsour.2009.09.001
(3) Zhang, T. S.; Ma, J.; Leng, Y. J.; Chan, S. H.; Hing, P.; Kilner, J. A. Solid State Ionics 2004, 168, 187.  doi: 10.1016/j.ssi.2004.02.015
(4) Duan, T.; Yan, X. M.; Liu, X. Y.; Bai, L.; Pei, Zheng, M. Z.; Zhu, C. J.; Wang, D. J.; Su, W. H. J. Power Sources 2010, 195, 6488.
(5) Molenda, J.; Swierczek, K.; Zajac, W. J. Power Sources 2007, 173, 660.
(6) Steele, B. C. H. Solid State Ionics 2000, 129, 95.  doi: 10.1016/S0167-2738(99)00319-7
(7) Jennifer, L. M. R.; Anna, I.; Ludwig,; J. G. Acta Mater 2006, 54, 1721.  doi: 10.1016/j.actamat.2005.11.032
(8) Gerhardt, R.; Nowick, A. S.; Mochel, M. E.; Dumler, I. J. Am. Ceram. Soc. 1986, 69, 641.  doi: 10.1111/j.1151-2916.1986.tb07464.x
(9) Guo, X.; Waser, R. Prog. Mater. Sci. 2006, 51, 151.  doi: 10.1016/j.pmatsci.2005.07.001
(10) Wojciech, Z.; Leopoldo, S.; Konrad, S.; Janina, M. J. Power Soures 2009, 194, 2.  doi: 10.1016/j.jpowsour.2008.12.020
(11) Zhang, T. S.; Ma, J.; Kong, L. B.; Hing, P.; Leng, Y. J.; Chan, S.H.; Kilner, J. A. J. Power Sources 2003, 124, 26.  doi: 10.1016/S0378-7753(03)00625-6
(12) Park, H. J.; Choi, G. M. Solid State Ionics 2008, 178, 1746.  doi: 10.1016/j.ssi.2007.12.003
(13) Xu, H. M.; Yan, H. G.; Chen, Z. H. Powder Metallurgy Technology 2008, 26, 443. [徐红梅, 严红革, 陈振华. 粉末冶金技术, 2008, 26, 443.]
(14) Zhang, T. S.; Ma, J.; Chan, S. H.; Kilner, J. A. Solid State Ionics 2005, 176, 377.  doi: 10.1016/j.ssi.2004.07.022
(15) Xu, D.; Liu, X. M.; Xu, S. F.; Yan, D. T.; Pei, L.; Zhu, C. J.; Wang, D. J.; Su, W. H. Solid State Ionics 2011, 192, 510.  doi: 10.1016/j.ssi.2010.03.026
(16) Zhang, T. S.; Ma, J.; Leng, Y. J.; Chan, S. H.; Hing, P.; Kilner, J. A. Solid State Ionics, 2004, 167, 203.  doi: 10.1016/j.ssi.2004.01.006
(17) Cho, P. S.; Cho, Y. H.; Park, S. Y.; Lee, S. B.; Kim, D. Y.; Park, H. M.; G. A.; J. D.; Lee, J. H. J. Electrochem. Soc. 2009, 3, 339.
(18) Yan, M.; Mori, T.; Zou, J.; Auchterlonie, G. J.; Drennan, J. J. Eur. Ceram. Soc. 2010, 30, 2505.  doi: 10.1016/j.jeurceramsoc.2010.04.036
(19) Li, B.; Wei, X.; Pan, W. J. Power Sources 2008, 183, 498.  doi: 10.1016/j.jpowsour.2008.05.050
(20) Cho, Y. H.; Cho, P. S.; Auchter, G.; Kim, D. K.; Lee, J. H.; Kim, D. Y.; Park, H. M.; Drennan, J. Acta Mater. 2007, 55, 4807.  doi: 10.1016/j.actamat.2007.05.001
(21) Wang, F. Y.; Wan, B. Z.; Cheng, S. J. Solid State Electrochem. 2005, 9, 168.  doi: 10.1007/s10008-004-0575-0
(22) Zheng, Y. F.; Zhou, M.; Ge, L.; Li, S. J.; Chen, H.; Guo, L. C. J. Alloy. Compd. 2011, 509, 546.  doi: 10.1016/j.jallcom.2010.09.103
(23) Zhang, T. S.; Hing P.; Huang, H. T.; Kilner, J. A. J. Mater. Sci. 2002, 37, 997.  doi: 10.1023/A:1014362000128
(24) McBride, J. R.; Hass, K. C.; Poindexter, B. D.; Weber, W. H.; J. Appl. Phys. 1994, 76, 2435.  doi: 10.1063/1.357593
(25) Dong, Q.; Du, Z. H.; Zhang, T. S.; Lu, J.; Song, X. C.; Ma, J. Int. J. Hydrog. Energy 2009, 34, 7908.
(26) Ma, Z. F.; Liang, G. C.; Liang, J. S. Acta Phys. -Chim. Sin. 2005, 21, 666. [马志芳, 梁广川, 梁金生. 物理化学学报, 2005, 21, 666.]

[1]	何子旭, 陈亚威, 黄凡洋, 揭育林, 李新鹏, 曹瑞国, 焦淑红. 氟代溶剂在锂金属电池中的应用[J]. 物理化学学报, 2022, 38(11): 2205005 - .
[2]	华广斌, 樊晏辰, 张千帆. 计算模拟在锂金属负极研究中的应用[J]. 物理化学学报, 2021, 37(2): 2008089 - .
[3]	杨毅, 闫崇, 黄佳琦. 锂电池中固体电解质界面研究进展[J]. 物理化学学报, 2021, 37(11): 2010076 - .
[4]	王晗, 安汉文, 单红梅, 赵雷, 王家钧. 全固态电池界面的研究进展[J]. 物理化学学报, 2021, 37(11): 2007070 - .
[5]	陈光海,白莹,高永晟,吴锋,吴川. 全固态钠离子电池硫系化合物电解质[J]. 物理化学学报, 2020, 36(5): 1905009 - .
[6]	徐来强,李佳阳,刘城,邹国强,侯红帅,纪效波. 无机钠离子电池固体电解质研究进展[J]. 物理化学学报, 2020, 36(5): 1905013 - .
[7]	蒋江民,聂平,董升阳,吴宇婷,张校刚. 预嵌锂用穿孔集流体对锂离子电容器电化学性能的影响[J]. 物理化学学报, 2017, 33(4): 780 -786 .
[8]	郑其格,刘惠,夏泉,刘青山,牟林. 两种疏水型膦类离子液体的密度、动力粘度及电导率[J]. 物理化学学报, 2017, 33(4): 736 -744 .
[9]	刘青山,刘惠,牟林. 1-丁腈-3-甲基咪唑双三氟甲基磺酸亚胺的性质[J]. 物理化学学报, 2016, 32(3): 617 -623 .
[10]	郑玲,潘懿,季宏祥,马晓雪,邢楠楠,关伟. 基于离子交换跃迁模型和实验法对离子液体Walden乘积的研究[J]. 物理化学学报, 2016, 32(11): 2663 -2670 .
[11]	刘兴蕊,严会娟,王栋,万立骏. 单晶硅片负极界面形貌的原位AFM探测[J]. 物理化学学报, 2016, 32(1): 283 -289 .
[12]	宿洪祯,尹静梅,刘青山,李长平. 四种深共融溶剂的性质:密度、电导率、动力粘度及折光率[J]. 物理化学学报, 2015, 31(8): 1468 -1473 .
[13]	汪秀萍, 周德凤, 杨国程, 孙世成, 李朝辉. Ce_0.8Nd_0.2O_1.9-La_0.95Sr_0.05Ga_0.9Mg_0.1O_3-δ固体复合电解质的结构和电性能[J]. 物理化学学报, 2014, 30(1): 95 -101 .
[14]	刘德治, 候西鑫, 朱秀玲, 王瑞, 井健, 崔悦. 基于自交联杂萘联苯聚芳醚阴离子交换膜制备及其物理化学性质[J]. 物理化学学报, 2013, 29(12): 2573 -2578 .
[15]	李长平, 李琢, 邹本雪, 刘青山, 刘晓霞. 质子型离子液体N,N-二甲基乙醇胺丙酸盐的密度、粘度及电导率[J]. 物理化学学报, 2013, 29(10): 2157 -2161 .

MgO或Fe₂O₃掺杂Ce_0.8Nd_0.2O_1.9固体电解质的结构和电性能

Structure and Electrical Properties of MgO or Fe₂O₃-Doped Ce_0.8Nd_0.2O_1.9 Solid Electrolytes

PDF

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

Metrics

推荐阅读 0