NH4+对甲酸在炭载Pd催化剂上氧化性能的影响

doi:10.3866/PKU.WHXB20101206

物理化学学报 >> 2010, Vol. 26 >> Issue (12): 3199-3202.doi: 10.3866/PKU.WHXB20101206

NH₄⁺对甲酸在炭载Pd催化剂上氧化性能的影响

李焕芝, 唐亚文, 陆天虹

南京师范大学化学与材料科学学院, 南京210097

收稿日期:2010-08-16 修回日期:2010-10-10 发布日期:2010-12-01
通讯作者: 陆天虹 E-mail:tianhonglu@263.net
基金资助:
国家自然科学基金(20873065, 21073094)资助项目

Effect of NH₄⁺ on the Electrocatalytic Performance of Carbon Supported Pd Catalyst for Formic Acid Oxidation

LI Huan-Zhi, TANG Ya-Wen, LU Tian-Hong

College of Chemistry and Material Science, Nanjing Normal University, Nanjing 210097, P. R. China

Received:2010-08-16 Revised:2010-10-10 Published:2010-12-01
Contact: LU Tian-Hong E-mail:tianhonglu@263.net
Supported by:
The project was supported by the National Natural Science Foundation of China (20873065, 21073094).

摘要/Abstract

摘要：

为了解HClO₄、NH₄ClO₄和NaClO₄电解液对炭载Pd(Pd/C)催化剂电极对甲酸氧化的电催化性能的影响, 在用X射线衍射(XRD)谱、能量色散谱(EDS)和透射电子显微镜(TEM)对Pd/C 催化剂进行表征的基础上,采用电化学方法测量了Pd/C催化剂在不同电解液中对甲酸氧化的电催化性能. 发现在不同电解液中, Pd/C催化剂对甲酸氧化的电催化活性和稳定性按NH₄ClO₄>NaClO₄>HClO₄的次序降低. 由于甲酸的存在, 不同电解液的pH相差较小, 因此, 电解液的pH影响较小, 而阳离子的影响较大. 在NaClO₄电解液中的性能优于在HClO₄电解液中的性能是pH的影响. 在NH₄ClO₄电解液中的性能优于在NaClO₄电解液中是由于NH₄⁺能降低CO在Pd/C催化剂电极上的吸附强度和吸附量, 这一发现对提高直接甲酸燃料电池(DFAFC)的性能很有意义.

关键词: 甲酸, 电解液, 钯, 直接甲酸燃料电池

Abstract:

We investigated the effect of HClO₄, NH₄ClO₄, and NaClO₄ electrolytes on the electrocatalytic performance of a Pd/C catalyst electrode for formic acid oxidation. The Pd/C catalyst was characterized by X-ray diffraction (XRD), energy dispersive spectroscopy (EDS), and transmission electron microscopy (TEM). The performance of the Pd/C catalyst electrode during formic acid oxidation in different electrolytes was measured using electrochemical methods. We found that the electrocatalytic activity and stability of the Pd/C catalyst electrode for formic acid oxidation decreased in the following order: NH₄ClO₄ > NaClO₄ > HClO₄. The difference in pH between the different electrolytes was small because of the presence of formic acid. Therefore, the electrolyte pH has a small effect and the cations have a large effect. The better performance of the NaClO₄ electrolyte compared to the HClO₄ electrolyte is due to a pH effect. The better performance of the NH₄ClO₄ electrolyte compared to the NaClO₄ electrolyte is due to NH₄⁺ decreasing the adsorption strength and amount of CO on the Pd/C catalyst. This finding has large significance for the increase in the performance of the direct formic acid fuel cell (DFAFC).

Key words: Formic acid, Electrolyte, Palladium, Direct formic acid fuel cell

MSC2000:

O643

李焕芝, 唐亚文, 陆天虹. NH₄⁺对甲酸在炭载Pd催化剂上氧化性能的影响[J]. 物理化学学报, 2010, 26(12): 3199-3202.

LI Huan-Zhi, TANG Ya-Wen, LU Tian-Hong. Effect of NH₄⁺ on the Electrocatalytic Performance of Carbon Supported Pd Catalyst for Formic Acid Oxidation[J]. Acta Phys. -Chim. Sin., 2010, 26(12): 3199-3202.

参考文献

1. Rhee, Y.; Ha, S.; Masel, R. I. J. Power Sources, 2003, 117: 35
2. Lu, T. H.; Tang, Y.W.; Zhang, L. L.; Gao, Y. Batt. Ind., 2007, 12: 412 [陆天虹, 唐亚文, 张玲玲, 高颖. 电池工业, 2007, 12: 412]
3. Ha, S.; Larsen, R.; Masel, R. I.;Waszczuk, P.;Wieckowski, A.; Barnard, T. J. Power Sources, 2002, 111: 83
4. Li, X. G.; Hsing, I. M.Electrochim. Acta, 2006, 51: 3477
5. Yu, X.W.; Pickup, P. G. J. Power Sources, 2009, 187: 493
6. Wang, X.; Hu, J. M.; Hsing, I. M. J. Electroanal. Chem., 2004, 562: 73
7. Ha, S.; Larsen, R.; Masel, R. I. J. Power Sources, 2005, 144: 28
8. Ha, S.; Larsen, R.; Zhu, Y. Fuel Cells, 2004, 4: 337
9. Wang, X.; Tang, Y.W.; Lu, T. H. Electrochemistry, 2008, 14: 6 [王新, 唐亚文, 陆天虹. 电化学, 2008, 14: 6]
10. Jiang, J. H.; Kucernak, A. Electrochim. Acta, 2009, 54: 4545
11. Chen, C. H.; Liou,W. J.; Lin, H. M.;Wu, S. H.; Mikolajczuk, A.; Stobinski, L.; Borodzinski, A.; Kedzierzawski, P.; Kurzydlowski, K. Phys. Status Solid A, 2010, 207: 1160
12. Wang, X. M.; Xia, Y. Y. Electrochem. Commun., 2008, 10: 1644
13. Matol?nova, I.; Fabk, S.; Masek, K. Vacuum, 2003, 71: 41
14. Wang, X.; Tang, Y.W.; Gao, Y.; Lu, T. H. J. Power Sources,2008, 175: 784
15. Yu, X.W.; Pickup, P. G. J. Power Sources, 2009, 192: 279
16. Yu, X.W.; Pickup, P. G. Electrochem. Commun., 2010, 12: 800
17. Cao, S.;Wang, Y. E.; Lu, T. H.; Tang, Y.W. Chin. J. Appl. Chem., 2009, 26: 613. [曹爽, 王彦恩, 陆天虹, 唐亚文. 应用化学, 2009, 26: 613]
18. Zhang, L. L.; Tang, Y.W.; Bao, J. C.; Lu, T. H.; Li, C. J. Power Sources, 2006, 162: 177
19. Yang, G. X.; Chen, Y.; Zhou, Y. M.; Tang, Y.W.; Lu, T. H. Electrochem. Commun., 2010, 12: 492
20. Wang, J. Y.; Kang, Y. Y.; Yang, H.; Cai,W. B. J. Phys. Chem. C, 2009, 113: 8366
21. Yang, G. X.; Deng, L. J.; Tang, Y.W.; Lu, T. H. Chem. J. Chin. Univ., 2009, 30: 1173. [杨改秀, 邓玲娟, 唐亚文, 陆天虹. 高等学校化学学报, 2009, 30: 1173]
22. Yang, G. X.; Chen, T. T.; Tang, Y.W.; Lu, T. H. Acta Phys. -Chim. Sin., 2009, 25: 2450. [杨改秀, 陈婷婷, 唐亚文, 陆天虹. 物理化学学报, 2009, 25: 2450]
23. Haan, J. L.; Masel, R. I. Electrochim. Acta, 2009, 54: 4073
24. Liao, C.;Wei, Z. D.; Chen, S. G.; Li, L.; Ji, M. B.; Tan, Y.; Liao, M. J. J. Phys. Chem. C, 2009, 113: 5705
25. Hoshi, N.; Kuroda, M.; Ogawa, T.; Koga, O.; Hori, Y. Langmuir,2004, 20: 5066
26. Feliu, J. M.; Herrero, E.//Vielstich,W.; Gasteiger, H. A.; Lamm, A. Handbook of fuel cells. New York:Wiley, 2003: 679

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NH₄⁺对甲酸在炭载Pd催化剂上氧化性能的影响

Effect of NH₄⁺ on the Electrocatalytic Performance of Carbon Supported Pd Catalyst for Formic Acid Oxidation

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