$La_xCe_{1-x}Co_yCu_{1-y}O_{3-{\alpha}}$ Perovskite촉매의 선택적 CO 산화반응에 관한 연구

Study on the Selective CO Oxidation Using $La_xCe_{1-x}Co_yCu_{1-y}O_{3-{\alpha}}$ Perovskite Catalysts

  • 강대규 (전북대학교 수소.연료전지공학과) ;
  • 이영일 (전북대학교 수소.연료전지공학과) ;
  • 손정민 (전북대학교 수소.연료전지공학과)
  • Kang, Dae-Kyu (Graduate School of Hydrogen Fuel Cells Engineering, Chonbuk National Univ.) ;
  • Lee, Young-Il (Graduate School of Hydrogen Fuel Cells Engineering, Chonbuk National Univ.) ;
  • Sohn, Jung-Min (Graduate School of Hydrogen Fuel Cells Engineering, Chonbuk National Univ.)
  • 발행 : 2007.03.15

초록

CO oxidation and selective CO oxidation of $La_xCe_{1-x}Co_yCu_{1-y}O_{3-{\alpha}}$ perovskite(x=1, 0.9, 0.7. 0.5; y=1, 0.9, 0.7, 0.5) were investigated. For CO oxidation, catalytic activities were studied according to different preparation conditions such as pH and calcination temperature. The influence of the change of the $O_2$ concentration for selective CO oxidation was studied, too. The substitution of Ce for La improved the catalytic activity for CO oxidation and selective CO oxidation and best activity was observed for $La_{0.7}Ce_{0.3}CoO_3$ prepared at pH 11 and calcined at $600^{\circ}C$. The temperature of 90% CO conversion for CO oxidation using $La_{0.7}Ce_{0.3}CoO_3$ was $230^{\circ}C$. In contrast to the enhancement effect by Ce substitution, the partial substitution of Cu for Co in $LaCo_yCu_{1-y}O_{3-{\alpha}}$ decreased catalytic activities for CO oxidation reaction compared to that using $LaCoO_3$. For selective CO oxidation, the best CO conversion was 66% at $230^{\circ}C$ for $La_{0.7}Ce_{0.3}CoO_3$. The CO conversion of $La_{0.7}Ce_{0.3}CoO_3$ was greatly increased from 66% to 91% as increasing $O_2$ concentration from 1% to 2%.

키워드

참고문헌

  1. C. S. Song, 'Fuel processing for low-temperature and high-temperature fuel cells challenges, and opportunities for sustainable development in the 21st century', Catalysis Today, Vol. 77, 2002, pp. 17-49 https://doi.org/10.1016/S0920-5861(02)00231-6
  2. I. H Son and A. M Lane, 'Promotion of Pt/$\Upsilon$ -$Al_{2}O_{3}$ by Ce for preferential oxidation of CO in H2', Catalysis Letters, Vol. 76, No. 3-4, 2001, pp. 151-154 https://doi.org/10.1023/A:1012293311973
  3. Y. Minemura, M. Kuriyama, S. Ito, K. Tomishige, and K. Kunimori, 'Additive effect of alkali metal ions on preferential CO oxidation over Pt/$Al_{2}O_{3}$', Catalysis communications, Vol. 7, No.9, 2006, pp. 623-626 https://doi.org/10.1016/j.catcom.2006.01.028
  4. A. Parinyaswan, S. Pongstabodee, and A. Luengnaruemitchal, 'Catalytic performances of Pt-Pd/$CeO_{2}$ catalysts for selective CO oxidation', International Journal of Hydrogen Energy, Vol. 31, No. 11, 2006, pp. 1942-1949 https://doi.org/10.1016/j.ijhydene.2006.05.002
  5. A. Holmgren, F. Azamoush, and E. Fridell, 'Influence of pre-treatment on the low-temperature activity of Pt/ceria', Applied Catalysis B: Environmental, Vol. 22, No.1, 1999, pp. 49-61 https://doi.org/10.1016/S0926-3373(99)00033-8
  6. W. Deng, J. De Jesus, H. Saltsburg, and M. Flytzani-Stephanopoulos, 'Low-content gold-ceria catalysts for the water-gas shift and preferential CO oxidation reactions', Applied Catalysis A, General, Vol. 291, No. 1-2, 2005, pp. 126-135 https://doi.org/10.1016/j.apcata.2005.02.048
  7. A. Luengnatuemitchi, D.T.K. Thoa, S. Osuwan, and E. Gulari, 'A comparative study of Au/$MnO_{x}$ and Au/$FeO_{x}$ catalysts for the catalytic oxidation of CO in hydrogen rich stream', International Journal of Hydrogen Energy, Vol. 30, No.9, 2005, pp. 981-987 https://doi.org/10.1016/j.ijhydene.2004.11.008
  8. C. K. Rhee, and H. I. Lee, 'CO oxidation on $LaCoO_{3}$ perovskite', Korean Journal of Chemical Engineering, Vol. 11, No.1, 1994, pp. 48-54 https://doi.org/10.1007/BF02697514
  9. S. H. Lee, J. Y. Lee, Y. M. Park, J. H. Wee, and K Y. Lee, 'Complete oxidation of methane and CO at low-temperature over $LaCoO_{3}$ prepared by spray-freezing freeze-drying method', Catalysis Today, Vol. 117, No. 1-3, 2006, pp. 376-381 https://doi.org/10.1016/j.cattod.2006.05.035
  10. X. Wu, and L. R. Radovic, 'Catalytic oxidation of carbon/carbon composite materials in the presence of potassitun and calcitun acetates', Carbon, vol. 43, No.2, 2005, pp. 333-344 https://doi.org/10.1016/j.carbon.2004.09.025
  11. 김영호, 이충균, 이화영, '$LaCoO_{3}$ perovskite 촉매상의 NO환원반응', 화학 공학, Vol. 29, No.5, 1991, pp. 596-605
  12. J. L. Ayastuy, M. P. Gonzalez-Marcos, A. G. Gutierrez-Ortiz, J. R. Gonzalez-Velasco, and M. A. Gutierrez-Ortiz, 'Selective CO oxidation over $Ce_{x}Zr_{1-x}O_{2}$ supported Pt catalysts', Catalysis Today, Vol. 116, No.3, 2006, pp. 391-399 https://doi.org/10.1016/j.cattod.2006.05.074
  13. XC. Zheng, SP. Wang, SR. Wang, SM. Zhang, WP. Huang, and SH. Wu, 'Copper oxide catalysts supported on ceria for low-temperature CO oxidation', Catalysis Communications, Vol. 5, No. 12, 2004, pp. 729-732 https://doi.org/10.1016/j.catcom.2004.09.008
  14. XC. Zheng, XL. Zhang, XY. Wang, SR. Wang, and SH. Wu, 'Preparation and characterization of CuO/$CeO_{2}$ catalysts and their applications in low-temperature CO oxidation', Applied Catalysis A: General, Vol. 295, No.2, 2005, pp. 142-149 https://doi.org/10.1016/j.apcata.2005.07.048
  15. J. Kirchnerova, M. Alifanti, and B. Delmon, 'Evidence of phase cooperation in the $LaCoO_{3}-CeO_{2}-Co_{3}O_{4}$catalytic system in relation to activity in methane combustion', Applied Catalysis A: General, Vol. 231, 2002, pp. 65-80 https://doi.org/10.1016/S0926-860X(01)00903-6
  16. Y. Zhang-Steenwinkel, J. Beckers, and A. Bliek, 'Surface properties and catalytic performance in CO oxidation of ceritun substituted lanthantun-manganese oxides', Applied Catalysis A: General, Vol. 235, No. 1-2, 2002, pp. 79-92 https://doi.org/10.1016/S0926-860X(02)00241-7
  17. I. H. Son, M. Sharnsuzzoha, A. M. Lane, 'Promotion of Pt/v-$Al_{2}O_{3}$ by New pretreatment for Low Temperature preferential oxidation of CO in $H_{2}$ for PEM Fuel Cells', Journal of catalysis, Vol. 210, No.2, pp. 460-465