中温固体氧化物燃料电池La1.6Sr0.4Ni1-xCuxO4阴极材料的制备及电化学性能

doi:10.3866/PKU.WHXB201206272

物理化学学报 >> 2012, Vol. 28 >> Issue (09): 2065-2070.doi: 10.3866/PKU.WHXB201206272

中温固体氧化物燃料电池La_1.6Sr_0.4Ni_1-xCu_xO₄阴极材料的制备及电化学性能

李强, 赵辉, 江瑞, 郭力帆

黑龙江大学化学化工与材料学院, 功能无机材料化学教育部重点实验室, 哈尔滨 150080

收稿日期:2012-05-21 修回日期:2012-06-26 发布日期:2012-08-02
通讯作者: 李强 E-mail:hematite1211@yahoo.com.cn
基金资助:
黑龙江省教育厅(12521396)资助项目

Synthesis and Electrochemical Properties of La_1.6Sr_0.4Ni_1-xCu_xO₄ as Cathode Materials for Intermediate Temperature Solid Oxide Fuel Cells

LI Qiang, ZHAO Hui, JIANG Rui, GUO Li-Fan

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, P. R. China

Received:2012-05-21 Revised:2012-06-26 Published:2012-08-02
Contact: LI Qiang E-mail:hematite1211@yahoo.com.cn
Supported by:
The project was supported by the Fund from Heilongjiang Educational Department, China (12521396).

摘要/Abstract

摘要：

采用甘氨酸-硝酸盐法合成了中温固体氧化物燃料电池阴极材料La_1.6Sr_0.4Ni_1-xCu_xO₄ (x=0.2, 0.4, 0.6,0.8), 利用X射线衍射(XRD)和扫描电子显微镜(SEM)对其结构和微观形貌进行了表征. 结果表明, 该阴极材料与固体电解质Ce_0.9Gd_0.1O_1.95(CGO)在1000 °C烧结时不发生化学反应, 且烧结4 h 后, 二者之间可形成良好的接触界面. 利用电化学交流阻抗谱技术对阴极材料的电化学性能进行研究, 结果显示, 当Cu离子掺杂量(x)为0.6 时, La_1.6Sr_0.4Ni_0.4Cu_0.6O₄阴极具有最小的极化电阻, 在空气中当测试温度为750 °C时, 极化电阻为0.35 Ω·cm². 在不同氧分压条件下电化学阻抗谱分析结果表明, 电极上的两个氧还原反应主要包含氧离子从三相界面向电解质CGO 转移的过程和电荷的迁移过程, 其中电荷的迁移过程为电极反应的速率控制步骤.La_1.6Sr_0.4Ni_0.4Cu_0.6O₄电极在空气中700 °C和阴极电流密度为45 mA·cm^-2时, 阴极过电位为45 mV. 本研究的初步结果表明La_1.6Sr_0.4Ni_1-xCu_xO₄材料是一种电化学性能较为优良的新型中温固体氧化物燃料电池(IT-SOFC)阴极材料.

关键词: 中温固体氧化物燃料电池, La_1.6Sr_0.4Ni_1-xCu_xO₄阴极材料, 甘氨酸-硝酸盐法, 电化学性能, 氧还原反应

Abstract:

Cathodic materials La_1.6Sr_0.4Ni_1-xCu_xO₄ (x=0.2, 0.4, 0.6, 0.8), for an intermediate temperature solid oxide fuel cell (IT-SOFC), were prepared by a glycine-nitrate process and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM). Results showed that no reaction occurred between the La_1.6Sr_0.4Ni_1-xCu_xO₄ electrode and the Ce_0.9Gd_0.1O_1.95 (CGO) electrolyte at 1000 °C, and that the electrode formed good contact with the electrolyte after sintering at 1000 °C for 4 h. Electrochemical AC impedance spectroscopy measurements were used to study cathodic performance. The La_1.6Sr_0.4Ni_0.4Cu_0.6O₄ cathode gave the lowest polarization resistance (R_p) of 0.35 Ω·cm² at 750 ° C in air. Electrode properties of La_1.6Sr_0.4Ni_1-xCu_xO₄ were studied under various temperatures and oxygen partial pressures. The two main oxygen reduction processes at the cathode are the oxygen ion transfer from the triple phase boundary to CGO electrolyte, and the charge transfer process. Charge transfer is the major rate limiting step for La_1.6Sr_0.4Ni_1-xCu_xO₄ cathode. The La_1.6Sr_0.4Ni_0.4Cu_0.6O₄ cathode exhibited the lowest overpotential, about 45 mV for a current density of 45 mA·cm^-2 at 700 °C in air. This preliminary work showed that the present La_1.6Sr_0.4Ni_1-xCu_xO₄ materials may be potential cathodes for use in IT-SOFCs.

Key words: Intermediate temperature solid oxide fuel cell, La_1.6Sr_0.4Ni_1-xCu_xO₄ cathode material, Glycine-nitrate process, Electrochemical property, Oxygen reduction reaction

李强, 赵辉, 江瑞, 郭力帆. 中温固体氧化物燃料电池La_1.6Sr_0.4Ni_1-xCu_xO₄阴极材料的制备及电化学性能[J]. 物理化学学报, 2012, 28(09), 2065-2070. doi: 10.3866/PKU.WHXB201206272

LI Qiang, ZHAO Hui, JIANG Rui, GUO Li-Fan. Synthesis and Electrochemical Properties of La_1.6Sr_0.4Ni_1-xCu_xO₄ as Cathode Materials for Intermediate Temperature Solid Oxide Fuel Cells[J]. Acta Phys. -Chim. Sin. 2012, 28(09), 2065-2070. doi: 10.3866/PKU.WHXB201206272

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201206272

https://www.whxb.pku.edu.cn/CN/Y2012/V28/I09/2065

参考文献

(1) Skinner, S. J.; Kilner, J. A. Solid State Ionics 2000, 135, 709.doi: 10.1016/S0167-2738(00)00388-X
(2) Ding, X. F.; Kong, X.; Jiang, J. G.; Cui, C. Int. J. Hydrog. Energy 2009, 34, 6869. doi: 10.1016/j.ijhydene.2009.06.041
(3) Peng, B.; Chen, G.;Wang, T.; Zhou, J.; Guo, J. J.; Cheng, Y. H.;Wu, K. J. Power Sources 2012, 201, 174.
(4) Taguchi, H. Mater. Res. Bull. 2001, 36, 1361. doi: 10.1016/S0025-5408(01)00631-6
(5) Vashook, V.; Girdauskaite, E.; Zosel, J.;Wen, T. L.; Ullmann,H.; Guth, U. Solid State Ionics 2006, 177, 1163. doi: 10.1016/j.ssi. 2006.05.018
(6) Minervini, L.; Grimes, R.W.; Kilner, J. A.; Sickafus, K. E.J. Mater. Chem. 2000, 10, 2349. doi: 10.1039/b004212i
(7) Yang, X. M.; Luo, L. T.; Zhong, H. Appl. Catal. A 2001, 207,69. doi: 10.1016/S0926-860X(00)00658-X
(8) Bochkov, D. M.; Kharton, V. V.; Kovalevsky, A. V.; Viskup, A.P.; Naumovich, E. N. Solid State Ionics 1999, 120, 281. doi: 10.1016/S0167-2738(99)00019-3
(9) Vashooka, V. V.; Trofimenko, N. E.; Ullmann, H.; Makhnach, L.V. Solid State Ionics 2000, 131, 329. doi: 10.1016/S0167-2738(00)00571-3
(10) Yang, J. F.; Cheng, J. G.; Fan, Y. M.;Wang, R.; Gao, J. F. Acta Phys. -Chim. Sin. 2012, 28, 1230. [杨俊芳, 程继贵, 樊玉萌,王睿, 高建峰. 物理化学学报, 2012, 28, 1230.] doi: 10.3866/PKU.WHXB201202232
(11) Khandale, A. P.; Bhoga, S. S. J. Power Sources 2010, 195, 7974.doi: 10.1016/j.jpowsour.2010.06.044
(12) Al Daroukh, M.; Vashook, V. V.; Ullmann, H.; Tietz, F.; ArualRaj, I. Solid State Ionics 2003, 158, 141. doi: 10.1016/S0167-2738(02)00773-7
(13) Jorgensen, J.; Dabrowski, B.; Pei, S.; Richards, D. R.; Hinks, D.G. Phys. Rev. B 1989, 40, 2187. doi: 10.1103/PhysRevB.40.2187
(14) Li, Q.; Fan, Y.; Zhao, H.; Huo, L. H. Chin. J. Inorg. Chem.2006, 22, 2025. [李强, 范勇, 赵辉, 霍丽华. 无机化学学报, 2006, 22, 2025.]
(15) Inprasit, T.; Limthongkul, P.;Wongkasemjit, S. ECS Transactions 2009, 25, 2581.
(16) Ling, Y. H.; Zhao, L.; Lin, B.; Dong, Y. C.; Zhang, X. Z.; Meng,G. Y.; Liu, X. Q. Int. J. Hydrog. Energy 2010, 35, 6905. doi: 10.1016/j.ijhydene.2010.04.021
(17) Zhang, H.;Wang, T.; Dong, X.; Lin,W. J. Nat. Gas Chem.2009, 18, 45. doi: 10.1016/S1003-9953(08)60084-5
(18) Zha, S.W.; Moore, A.; Abernathy, H.; Liu, M. L.J. Electrochem. Soc. 2004, 151, A1128.
(19) Zhao, H.; Li, Q.; Sun, L. P. Sci. China Ser. B-Chem. 2011, 54,898. doi: 10.1007/s11426-011-4290-2
(20) Aguadero, A.; Alonso, J. A.; Escudero, M. J.; Daza, L. Solid State Ionics 2008, 151, 393.
(21) Li, Q.; Zhao, H.; Huo, L. H.; Sun, L. P.; Cheng, X. L.; Grenier,J. C. Electrochem. Commun. 2007, 9, 1508. doi: 10.1016/j.elecom.2007.02.013
(22) Li, Q.; Fan, Y.; Zhao, H.; Sun, L. P.; Huo, L. H. J. Power Sources 2007, 167, 64. doi: 10.1016/j.jpowsour.2007.02.018
(23) Efimov, K.; Halfer, T.; Kuhn, A.; Heitjans, P.; Caro, J.; Feldhoff,A. Chem. Mater. 2010, 22, 1540. doi: 10.1021/cm902882s
(24) Irvine, J. T. S.; Sinclair, D. C.;West, A. R. Adv. Mater. 1990, 2,132. doi: 10.1002/adma.19900020304
(25) Takeda, Y.; Kanno, R.; Noda, M.; Yamamoto, O.J. Electrochem. Soc. 1987, 134, A2656.
(26) Sicbeit, E.; Hammouche, A.; Kleitz, M. Electrochim. Acta 1995,40, 1741. doi: 10.1016/0013-4686(94)00361-4
(27) Li, Q.; Zeng, X.; Sun, L. P.; Zhao, H.; Huo, L. H.; Grenier, J. C.Int. J. Hydrog. Energy 2012, 37, 2552. doi: 10.1016/j.ijhydene.2011.11.014
(28) Mauvy, F.; Lalanne, C.; Bassat, J. M.; Grenier, J. C.; Zhao, H.;Dordor, P.; Stevens, P. J. Eur. Ceram. Soc. 2005, 25, 2669.doi: 10.1016/j.jeurceramsoc.2005.03.120

[1]	于彦会, 饶鹏, 封苏阳, 陈民, 邓培林, 李静, 苗政培, 康振烨, 沈义俊, 田新龙. 钴原子团簇用于高效氧还原反应[J]. 物理化学学报, 2023, 39(8): 2210039 -0 .
[2]	陈帅, 余创, 罗启悦, 魏超超, 李莉萍, 李广社, 程时杰, 谢佳. 卤化物固态电解质研究进展[J]. 物理化学学报, 2023, 39(8): 2210032 -0 .
[3]	兰畅, 楚宇逸, 王烁, 刘长鹏, 葛君杰, 邢巍. 质子交换膜燃料电池阴极非贵金属M-N_x/C型氧还原催化剂研究进展[J]. 物理化学学报, 2023, 39(8): 2210036 -0 .
[4]	彭林峰, 余创, 魏超超, 廖聪, 陈帅, 张隆, 程时杰, 谢佳. 锂硫银锗矿固态电解质研究进展[J]. 物理化学学报, 2023, 39(7): 2211034 -0 .
[5]	齐亚娥, 夏永姚. 电解液调控策略提升水系锌离子电池正极材料电化学性能[J]. 物理化学学报, 2023, 39(2): 2205045 -0 .
[6]	李景学, 于跃, 徐斯然, 闫文付, 木士春, 张佳楠. 电子自旋效应在电催化剂中的作用[J]. 物理化学学报, 2023, 39(12): 2302049 - .
[7]	莫英, 肖逵逵, 吴剑芳, 刘辉, 胡爱平, 高鹏, 刘继磊. 锂离子电池隔膜的功能化改性及表征技术[J]. 物理化学学报, 2022, 38(6): 2107030 - .
[8]	薄拯, 孔竞, 杨化超, 郑周威, 陈鹏鹏, 严建华, 岑可法. 基于混合溶剂有机电解液的超低温孔洞石墨烯超级电容[J]. 物理化学学报, 2022, 38(4): 2005054 - .
[9]	刘苗苗, 杨茅茂, 舒欣欣, 张进涛. 燃料电池碳基氧还原催化剂的设计与应用[J]. 物理化学学报, 2021, 37(9): 2007072 - .
[10]	韩洪仨, 王彦青, 张云龙, 丛媛媛, 秦嘉琪, 高蕊, 柴春晓, 宋玉江. 金属卟啉修饰的多孔聚苯胺基氧还原电催化剂[J]. 物理化学学报, 2021, 37(9): 2008017 - .
[11]	梁嘉顺, 刘轩, 李箐. 提升燃料电池铂基催化剂稳定性的原理、策略与方法[J]. 物理化学学报, 2021, 37(9): 2010072 - .
[12]	李峥嵘, 申涛, 胡冶州, 陈科, 陆贇, 王得丽. 有序金属间化合物电催化剂在燃料电池中的应用进展[J]. 物理化学学报, 2021, 37(9): 2010029 - .
[13]	丁亮, 唐堂, 胡劲松. 基于金属-氮-碳结构催化剂的质子交换膜燃料电池研究进展[J]. 物理化学学报, 2021, 37(9): 2010048 - .
[14]	高增强, 王聪勇, 李俊俊, 朱亚廷, 张志成, 胡文平. 导电金属有机框架材料在电催化中的成就，挑战和机遇[J]. 物理化学学报, 2021, 37(7): 2010025 - .
[15]	肖瑶, 裴煜, 胡一帆, 马汝广, 王德义, 王家成. 磷化钴封装在磷富集的三维多孔碳及其双功能氧电催化性能研究[J]. 物理化学学报, 2021, 37(7): 2009051 - .

中温固体氧化物燃料电池La_1.6Sr_0.4Ni_1-xCu_xO₄阴极材料的制备及电化学性能

Synthesis and Electrochemical Properties of La_1.6Sr_0.4Ni_1-xCu_xO₄ as Cathode Materials for Intermediate Temperature Solid Oxide Fuel Cells

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