Preparation of Porous Carbon Fiber by Using MgO Powder and Its Characteristics of Catalysts for Fuel Cell

MgO를 이용한 다공성 탄소 섬유 제조 및 이를 이용한 연료전지용 촉매 특성

  • Nam, Kidon (Advanced Fuel Cell Research Center, Korea Institute of Energy Research) ;
  • Kim, Sang-Kyung (Advanced Fuel Cell Research Center, Korea Institute of Energy Research) ;
  • Lim, Seongyop (Advanced Fuel Cell Research Center, Korea Institute of Energy Research) ;
  • Peck, Donghyun (Advanced Fuel Cell Research Center, Korea Institute of Energy Research) ;
  • Lee, Byoungrok (Advanced Fuel Cell Research Center, Korea Institute of Energy Research) ;
  • Jung, Doohwan (Advanced Fuel Cell Research Center, Korea Institute of Energy Research)
  • 남기돈 (한국에너지기술연구원 신연료전지센터) ;
  • 김상경 (한국에너지기술연구원 신연료전지센터) ;
  • 임성엽 (한국에너지기술연구원 신연료전지센터) ;
  • 백동현 (한국에너지기술연구원 신연료전지센터) ;
  • 이병록 (한국에너지기술연구원 신연료전지센터) ;
  • 정두환 (한국에너지기술연구원 신연료전지센터)
  • Received : 2008.09.05
  • Accepted : 2008.10.24
  • Published : 2008.12.31

Abstract

Nano-structured porous carbon fiber(PCF) for the catalyst supports of the direct methanol fuel cell (DMFC) were prepared from the mesophase pitch by using the nano-MgO powders. Specific surface area of the PCFs was $8{\sim}58m^2/g$ and surface pore structures had almost meso pore diameter of 10~20 nm which were depending on the amount of MgO spheres. Aqueous reduction method was used to load 60 wt% PtRu on the prepared PCF supports. The electro-oxidation activity and single cell performance of the 60 wt% Pt-Ru catalysts were measured by cyclic voltammetry and unit cell test. The performances of these catalysts increased by 5~10% compared with one of commercial catalyst.

Nano-MgO와 메조페이스 피치로부터 복합 탄소섬유를 만들고 MgO를 제거함으로써 직접 메탄올 연료전지용 촉매 담지체로서의 다공성 탄소섬유를 제조하였다. 이 다공성 탄소섬유의 비표면적은 $8{\sim}58m^2/g$ 이고, 표면기공구조는 마이크로기공이 거의 없이 MgO 입자크기 유래의 메조기공(10~15 nm)으로 구성된 것이 특징이며, MgO 혼입량(1~10 wt%)에 따라 조절할 수 있었다. 본 다공성 탄소섬유를 담지체로 이용하여 함침법으로 60 wt% Pt-Ru 촉매를 담지하였으며, 제조된 Pt-Ru 촉매의 메탄올 산화 특성 및 단위전지 성능 측정 결과 상용촉매에 비하여 5~10% 이상 향상된 값을 나타내었다

Keywords

Acknowledgement

Supported by : 지식경제부

References

  1. Joo, S. H., Choi, S. J., Oh, I. W., Kwak, J. H., Liu, Z., Terasaki, O. and Ryoo, R., 'Ordered Nanoporous Arrays of Carbon Supporting High Dispersions of Platinum Nanoparticles,' Nature, 412(6843), 169-172(2001)
  2. Han, S. J., Sohn, K. N. and Hyeon, T. H., 'Fabrication of New Nanoporous Carbons through Silica Templates and Their Application to the Adsorption of Bulky Dyes,' Chem. Mater., 12(11), 3337-3341(2000) https://doi.org/10.1021/cm000106t
  3. Hong, E. H., Jung, Y. H. and Lee, K. H., 'Preparation of Mesoporous Activated Carbon Fibers by Catalytic Gasification,' Korean J. Chem. Eng., 17(2), 237-240(2000) https://doi.org/10.1007/BF02707149
  4. Yim, K. S., Eom, S. Y., Ryu, S. K. and Edie, D. D., 'Microporosity and Behaviors of Metal Particles in Metal (Ag, Cu, Co)-Containing Activated Carbon Fibers,' HWAHAK KONGHAK, 41(4), 503-508(2003)
  5. Lim, S. Y., Hong, S. H., Qiao, W., Duayne Whitehurst, D., Yoon, S. H., Mochida, I., An, B. and Yokogawa, K., 'Carbon Nanofibers with Radially Oriented Channels,' Carbon, 45(1), 173-179(2007) https://doi.org/10.1016/j.carbon.2006.07.009
  6. Cho, T. H., Kim, S. Y., Cho, K. H. and Ryu, S. K., 'Melt-spinning of Silver-containing Precursor Pitches,' HWAHAK KONGHAK, 38(3), 338-342(2000)
  7. Ryu, S. K., Eom, S. Y., Yim, K. S. and Edie, D. D., 'Pore Characteristics of $TiO_2$-Containing Activated Carbon Fibers,' Korean Chem. Eng. Res., 42(3), 288-295(2004)
  8. Basova, Y. V., Edie, D. D., Badheka, P. Y. and Bellam, H. C., 'The Effect of Precursor Chemistry and Preparation Conditions on the Formation of Pore Structure in Metal-containing Carbon Fibers,' Carbon, 43(7), 1533-1545(2005) https://doi.org/10.1016/j.carbon.2005.01.041
  9. Hyeon, T. H., Han, S. J., Sung, Y. E., Park, K. W. and Kim, Y. W., 'High-Performance Direct Methanol Fuel Cell Electrodes using Solid-Phase-Synthesized Carbon Nanocoils,' Angewandte Chemie-International Edition, 42(36), 4352-4356(2003) https://doi.org/10.1002/anie.200250856
  10. Jung, D. H., Jung, J. H., Hong, S. H., Peck, D. H., Shin, D. R. and Kim, E. S., 'Characteristics of Pt-Ru Catalyst Supported on Activated Carbon for Direct Methanol Fuel Cell,' Carbon Science, 4(3), 121-125(2003)
  11. Park, G. G., Yang, T. H., Yoon, Y. G., Lee, W. Y. and Kim, C. S., 'Pore Size Effect of the DMFC Catalyst Supported on Porous Materials,' International Journal of Hydrogen Energy, 28, 645-650(2003) https://doi.org/10.1016/S0360-3199(02)00140-4
  12. Lee, J. B., Park, Y. K., Yang, O. B., Kang, Y. K., Jun, K. W., Lee, Y. J., Kim, H. Y., Lee, K. H. and Choi, W. C., 'Synthesis of Porous Carbons having Surface Functional Groups and Their Application to Direct-Methanol Fuel Cells,' J. Power Sources, 158(2), 1251-1255(2006) https://doi.org/10.1016/j.jpowsour.2005.10.085
  13. Liu, H., Song, C., Zhang, L., Zhang, J., Wang, H. and Wilkinson, D. P., 'A Review of Anode Catalysis in the Direct Methanol Fuel Cell,' J. Power Sources, 155(2), 95-110(2006) https://doi.org/10.1016/j.jpowsour.2006.01.030
  14. Mora, E., Blanco, C., Prada, V., Santamaria, R., Granda, M. and Menendez, R., 'A Study of Pitch-Precursors for General Purpose Carbon Fibres,' Carbon, 40(14), 2719-2725(2002) https://doi.org/10.1016/S0008-6223(02)00185-9
  15. Edie, D. D. and Dunham, M. G., 'Melt Spinning Pitch-based Carbon Fibers,' Carbon, 27(5), 647-655(1989) https://doi.org/10.1016/0008-6223(89)90198-X
  16. Nam, K. D., Kim, T. J., Kim, S. K., Lee, B. R., Peck, D. H., Ryu, S. K. and Jung, D. H., 'Preparation of Uniform Porous Carbon from Mesophase Pitch and Its Characteristics of Catalyst Support for the Direct Methanol Fuel Cell,' J. Korean Ind. Eng. Chem., 17(2), 223-228(2006)
  17. Korai, Y., Ishida, S., Watanabe, F., Yoon, S. H., Wang, Y. G., Mochida, I., Kato, I., Nakamura, T., Sakai, Y. and Komatsu, M., 'Preparation of Carbon Fiber from Isotropic Pitch Containing Mesophase Spheres,' Carbon, 35(12), 1733-1737(1997) https://doi.org/10.1016/S0008-6223(97)00128-0
  18. Ryu, S. K., Eom, S. Y., Cho, T. H. and Edie, D. D., 'Distribution of Silver Particles in Silver-containing Activated Carbon Fibers,' Carbon Science, 4(4), 168-174(2003)
  19. Gergg, S. J. and Sing, K. S. W., Adsorption, Surface Area and Porosity, 2nd ed., Academic Press Inc., New York, NY(1982)
  20. Sing, K. S. W., Everett, D. H., Haul, R. A. W., Moscou, L., Pierotti, R. A., Rouquerol, J. and Siemieniewska, T., 'Reporting Physisorption Data for Gas/Solid Systems with Special Reference to the Determination of Surface Area and Porosity,' Pure & Appl. Chem., 57(4), 603-619(1985) https://doi.org/10.1351/pac198557040603
  21. Lee, C. H., Lee, C. W., Kim, D. I., Jung, D. H., Kim, C. S. and Shin, D. R., 'Electrooxidation of Methanol on Pt-Ru Catalysts Supported by Basal Plane Graphite in Phosphoric Acid Solution,' J. Power Sources, 86(1-2), 478-481(2000) https://doi.org/10.1016/S0378-7753(99)00442-5
  22. Hyun, M. S., Kim, S. K., Lee, B. R., Peck, D. H., Shul, Y. G. and Jung, D. H., 'Effect of $NaBH_4$ Concentration on the Characteristics of PtRu/C Catalyst for the Anode of DMFC Prepared by the Impregnation Method,' Catalysis Today, 132(1-4), 138-145(2008) https://doi.org/10.1016/j.cattod.2007.12.034
  23. Antolini, E and Cardellini, F., 'Formation of Carbon Supported PtRu Alloys: an XRD Analysis,' J. Alloys and Compounds, 315(1-2), 118-122(2001) https://doi.org/10.1016/S0925-8388(00)01260-3
  24. Cattaneo, C., Sanchez, M. I. de Pinto, Mishima, H. Lopez, B. A. de Mishima, Lescano, D. and Cornaglia, L., 'Characterization of Platinum-rutheniun Electrodeposits using XRD, AES and XPS Analysis,' J. Electroanalytical Chem., 461(1-2), 32-39(1999) https://doi.org/10.1016/S0022-0728(98)00196-X
  25. Edie. D. D., 'The Effect of Processing on the Structure and Properties of Carbon Fibers,' Carbon, 36(4), 345-362(1998) https://doi.org/10.1016/S0008-6223(97)00185-1