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

引用本文: 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, doi: 10.3866/PKU.WHXB201206272 shu

Citation: 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 Physico-Chimica Sinica, doi: 10.3866/PKU.WHXB201206272 shu

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

基金项目:
黑龙江省教育厅(12521396)资助项目 (12521396)

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(C )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C 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:

English

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

1.
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, P. R. China
Received Date: 21 May 2012
Available Online: 02 August 2012
Fund Project:
黑龙江省教育厅(12521396)资助项目

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 (C ) electrolyte at 1000 °C, and that the electrode formed od 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 C 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

1. [1]
  
  (1) Skinner, S. J.; Kilner, J. A. Solid State Ionics 2000, 135, 709.doi: 10.1016/S0167-2738(00)00388-X
  (1) Skinner, S. J.; Kilner, J. A. Solid State Ionics 2000, 135, 709.doi: 10.1016/S0167-2738(00)00388-X
2. [2]
  (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(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. [3]
  (3) Peng, B.; Chen, G.;Wang, T.; Zhou, J.; Guo, J. J.; Cheng, Y. H.;Wu, K. J. Power Sources 2012, 201, 174.(3) Peng, B.; Chen, G.;Wang, T.; Zhou, J.; Guo, J. J.; Cheng, Y. H.;Wu, K. J. Power Sources 2012, 201, 174.
4. [4]
  (4) Taguchi, H. Mater. Res. Bull. 2001, 36, 1361. doi: 10.1016/S0025-5408(01)00631-6(4) Taguchi, H. Mater. Res. Bull. 2001, 36, 1361. doi: 10.1016/S0025-5408(01)00631-6
5. [5]
  (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(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. [6]
  (6) Minervini, L.; Grimes, R.W.; Kilner, J. A.; Sickafus, K. E.J. Mater. Chem. 2000, 10, 2349. doi: 10.1039/b004212i(6) Minervini, L.; Grimes, R.W.; Kilner, J. A.; Sickafus, K. E.J. Mater. Chem. 2000, 10, 2349. doi: 10.1039/b004212i
7. [7]
  (7) Yang, X. M.; Luo, L. T.; Zhong, H. Appl. Catal. A 2001, 207,69. doi: 10.1016/S0926-860X(00)00658-X(7) Yang, X. M.; Luo, L. T.; Zhong, H. Appl. Catal. A 2001, 207,69. doi: 10.1016/S0926-860X(00)00658-X
8. [8]
  (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(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. [9]
  (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(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. [10]
  (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(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. [11]
  (11) Khandale, A. P.; Bhoga, S. S. J. Power Sources 2010, 195, 7974.doi: 10.1016/j.jpowsour.2010.06.044(11) Khandale, A. P.; Bhoga, S. S. J. Power Sources 2010, 195, 7974.doi: 10.1016/j.jpowsour.2010.06.044
12. [12]
  (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(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. [13]
  (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(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. [14]
  (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.](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. [15]
  (15) Inprasit, T.; Limthongkul, P.;Wongkasemjit, S. ECS Transactions 2009, 25, 2581.(15) Inprasit, T.; Limthongkul, P.;Wongkasemjit, S. ECS Transactions 2009, 25, 2581.
16. [16]
  (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(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. [17]
  (17) Zhang, H.;Wang, T.; Dong, X.; Lin,W. J. Nat. Gas Chem.2009, 18, 45. doi: 10.1016/S1003-9953(08)60084-5(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. [18]
  (18) Zha, S.W.; Moore, A.; Abernathy, H.; Liu, M. L.J. Electrochem. Soc. 2004, 151, A1128.(18) Zha, S.W.; Moore, A.; Abernathy, H.; Liu, M. L.J. Electrochem. Soc. 2004, 151, A1128.
19. [19]
  (19) Zhao, H.; Li, Q.; Sun, L. P. Sci. China Ser. B-Chem. 2011, 54,898. doi: 10.1007/s11426-011-4290-2(19) Zhao, H.; Li, Q.; Sun, L. P. Sci. China Ser. B-Chem. 2011, 54,898. doi: 10.1007/s11426-011-4290-2
20. [20]
  (20) Aguadero, A.; Alonso, J. A.; Escudero, M. J.; Daza, L. Solid State Ionics 2008, 151, 393.(20) Aguadero, A.; Alonso, J. A.; Escudero, M. J.; Daza, L. Solid State Ionics 2008, 151, 393.
21. [21]
  (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(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. [22]
  (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(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. [23]
  (23) Efimov, K.; Halfer, T.; Kuhn, A.; Heitjans, P.; Caro, J.; Feldhoff,A. Chem. Mater. 2010, 22, 1540. doi: 10.1021/cm902882s(23) Efimov, K.; Halfer, T.; Kuhn, A.; Heitjans, P.; Caro, J.; Feldhoff,A. Chem. Mater. 2010, 22, 1540. doi: 10.1021/cm902882s
24. [24]
  (24) Irvine, J. T. S.; Sinclair, D. C.;West, A. R. Adv. Mater. 1990, 2,132. doi: 10.1002/adma.19900020304(24) Irvine, J. T. S.; Sinclair, D. C.;West, A. R. Adv. Mater. 1990, 2,132. doi: 10.1002/adma.19900020304
25. [25]
  (25) Takeda, Y.; Kanno, R.; Noda, M.; Yamamoto, O.J. Electrochem. Soc. 1987, 134, A2656.(25) Takeda, Y.; Kanno, R.; Noda, M.; Yamamoto, O.J. Electrochem. Soc. 1987, 134, A2656.
26. [26]
  (26) Sicbeit, E.; Hammouche, A.; Kleitz, M. Electrochim. Acta 1995,40, 1741. doi: 10.1016/0013-4686(94)00361-4(26) Sicbeit, E.; Hammouche, A.; Kleitz, M. Electrochim. Acta 1995,40, 1741. doi: 10.1016/0013-4686(94)00361-4
27. [27]
  (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(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. [28]
  (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
  (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

扫一扫看文章

计量

PDF下载量: 889
文章访问数: 2600
HTML全文浏览量: 68

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

English

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

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处