γ-Al2O3에 담지된 Cu-Mn 산화물 촉매의 활성 및 특성

Activity and Characteristics of Cu-Mn Oxide Catalysts Supported on γ-Al2O3

  • Kim, Hye-jin (Department of Environmental Science, Keimyung University) ;
  • Choi, Sung-Woo (Department of Environmental Science, Keimyung University) ;
  • Lee, Chang-Seop (Department of Chemistry, Keimyung University)
  • 투고 : 2005.09.29
  • 심사 : 2006.03.27
  • 발행 : 2006.04.30

초록

${\gamma}-Al_2O_3$에 담지한 Cu-Mn 산화물 촉매에서 톨루엔 완전산화 반응을 $160{\sim}280^{\circ}C$의 온도 범위에서 고정층 반응기로 조사하였다. BET, SEM, TPR, TPO, XPS 및 XRD를 이용하여 촉매 특성분석을 하였다. 톨루엔의 완전산화 반응은 $280^{\circ}C$ 이하에서 이루어졌으며, 적절한 Cu-Mn 담지량은 15.0 wt%Cu-10.0 wt%Mn인 것으로 나타났다. TPR/TPO 및 XPS 분석 결과, 15 Cu-10 Mn 촉매의 산화환원 봉우리가 낮은 온도로 이동하였으며 결합에너지가 높은 값으로 이동하였다. XRD 결과, 고분산된 Mn 산화물과 CuO 보다 $Cu_{1.5}Mn_{1.5}O_4$의 촉매활성 인자로서의 역할이 더욱 우수한 것으로 추측되며, 촉매의 활성은 촉매의 산화환원 능력과 촉매의 높은 산화 상태에 기인하는 것으로 사료된다.

The catalytic oxidation of toluene over $-Al_2O_3$ supported copper-manganese oxide catalysts in the temperature range of $160-280^{\circ}C$ was investigated by employing a fixed bed flow reactor. The catalysts were characterized by BET, scanning electron microscopy (SEM), temperature-programmed reduction(TPR), temperature-programmed oxidation(TPO), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction(XRD) techniques. Catalytic oxidation of toluene was achieved at the below $280^{\circ}C$, and the optimal content of copper and manganese in the catalyst was found to be 15.0 wt%Cu-10.0 wt%Mn. From the TPR/TPO and XPS results, the redox peak of 15 Cu-10 Mn catalyst shifted to the lower temperature, and the binding energy was shifted to the higher binding energy. Furthermore, It is considered that $Cu_{1.5}Mn_{1.5}O_4$ is superior to Mn oxides and CuO in the role as active factor of catalysts from the XRD results and also catalytic activities are dependent on the redox ability and high oxidation state of catalysts.

키워드

과제정보

연구 과제 주관 기관 : 한국산업기술재단

참고문헌

  1. Soichiro, S., J. Env. Hi-Tech., 9, 15-19(2004)
  2. Cooper, C. D., Alley, F. C., Air Pollution Control, 2nd ed., Waveland Press, 337(1994)
  3. Ihm, S. K., Jun, Y. D., Kim, D. C. and Jeong, K. E., 'Low-temperature Deactivation and Oxidation State of $Pd/-Al_2O_3$ Catalysts for Total Oxidation of n-hexane,' Catal. Today, 93(95), 149-154(2004) https://doi.org/10.1016/j.cattod.2004.06.096
  4. Centeno, M. A., Paulis, M., Montes, M. and Odriozola, J. A., 'Catalytic Combustion of Volatile Organic Compounds on Au/ $CeO_2/Al_2O_3$ and $Au/Al_2O_3$ Catalysts,' Appl. Catal. A:Gen., 234, 65-78(2002) https://doi.org/10.1016/S0926-860X(02)00214-4
  5. Li, W. B., Chu, W. B., Zhuang, M. and Hua, J., 'Catalytic Oxidation of Toluene on Mn-Containing Mixed Oxides Prepared in Reverse Microemulsions,' Catal. Today, 93(95), 205-209(2004) https://doi.org/10.1016/j.cattod.2004.06.042
  6. Mazzocchia, C. and Kaddouri, A., 'On the Activity of Copper Chromite Catalysts in Ethyl Acetate Combustion in the Presence and Absence of Oxygen,' J. Mol. Catal. A:Chem., 204(205), 647-654(2003) https://doi.org/10.1016/S1381-1169(03)00348-0
  7. Terribile, D., Trovarelli, A., Leitenburg, C. D., Primavera, A. and Dolcetti, G., 'Catalytic Combustion of Hydrocarbons with Mn and Cu-doped Ceria-zirconia Solid Solutions,' Catal. Today, 47, 133-140(1999) https://doi.org/10.1016/S0920-5861(98)00292-2
  8. Kim, S. C., 'The Catalytic Oxidation of Aromatic Hydrocarbons over Supported Metal Oxide,' J. Haz. Mat., B91, 285-299(2002)
  9. Papavasiliou, J., Avgouropoulos, G. and Ioannides, T., 'Steam Reforming Over Copper-manganese Spinel Oxide Catalysts,' Catal. Com., 6, 497-501(2005) https://doi.org/10.1016/j.catcom.2005.04.015
  10. Cheon, T. J., Kim, H. J. and Choi, S. W., 'Toluene Catalytic Oxidation by Manganese Oxide: (1) Activity and Characterization,' J. Korean. Soc. Atmos. Env., 21(2), 161-168(2005)
  11. Alonso, L., Palacios, J. M., Garcia, E. and Moliner, R., 'Characterization of Mn and Cu Oxides as Regenerable Sorbents for Hot Coal Gas Desulfurization,' Fuel Proc. Tech., 62, 31-44(2000) https://doi.org/10.1016/S0378-3820(99)00063-6
  12. Tang, X., Li, Y., Huang, X., Xu, Y., Zhu, H., Wang, J. and Shen, W., '$MnOx-CeO_2$ Mixed Oxide Catalysts for Complete Oxidation of Formaldehyde: Effect of Preparation Method and Calcination Temperature,' Appl. Catal. B:Env., 62, 265-273(2005) https://doi.org/10.1016/j.apcatb.2005.08.004
  13. Kim, Y. H. and Lee, H. I., 'Redox Property of Transition Metal Oxides in Catalytic Oxidation,' J. Korean. Ind. Eng. Chem., 10(8), 1161-1168(1999)
  14. Chon, H. Z. and Seo, G., Catalysis an Introduction, 4rd ed., Hanlimwon, Seoul(2002)
  15. http://www.lasurface.com
  16. Niemantsverdriet, J. W., Spectroscopy in Catalysis, second., Netherlands(2000)
  17. Wang, C. H., '$Al_2O_3$-Supportsd Transition-Metal Oxide Catalysts for Catalytic Incineration of Toluene,' Chemosphere, 55, 11-17(2004) https://doi.org/10.1016/j.chemosphere.2003.10.036