Catalytic Oxidation of Toluene over Mn-Ce/${\gamma}-Al_2O_3$ Catalyst Doped with Ce

Ce가 첨가된 Mn-Ce/${\gamma}-Al_2O_3$ 촉매상에서 톨루엔의 촉매 산화 반응

  • Cheon, Tae-Jin (Department of Environmental Science and Engineering, Keimyung University) ;
  • Kim, Hye-Jin (Department of Environmental Science and Engineering, Keimyung University) ;
  • Choi, Sung-Woo (Department of Environmental Science and Engineering, Keimyung University)
  • Published : 2005.05.31

Abstract

Catalytic oxidation of toluene on the manganese oxide catalysts and manganese-cerium oxide catalysts was investigated. The catalysts were characterised by X-ray diffraction(XRD), thermo gravimetric analyzer(TGA), toluene-temperature program reduction(Toluene-TPR). We found that the optimal manganese content was 18.2 wt.% and the optimal cerium content was 10.0 wt.% at catalytic oxidation of toluene. It is shown that ceria improves the activity of manganese oxide phases. From the XRD results, it was estimated that $MnO_2$ phase was active site in the monometallic and bimetallic catalysts. From the TGA and Toluene-TPR results, it show that ceria improves the mobility of the lattice oxygen, adequate oxidation state of the active phase, reduction ability at low temperature, and re-oxidation of the active site.

망간 산화물 촉매, 망간-세륨 산화물 촉매에서 톨루엔의 촉매 산화에 대하여 조사 하였다. XRD, TGA, 톨루엔-TPR 분석을 통해 촉매의 특성을 조사하였다. 톨루엔 산화반응에 있어서 망간 18.2 wt.% 세륨 10.0 wt.%이 적절한 비율인 것으로 나타났다. 그리고 세리아가 망간 산화물에서의 활성을 증진 시키는 것으로 보여진다. XRD결과 $MnO_2$가 황성 자리인 것으로 추측된다. TGA 톨루엔-TPR결과 세리아가 격자 산소의 이동성, 활성자리의 적절한 상화 상태, 저온에서의 환원능력 및 활성자리의 재산화 능력을 증진시키는 것으로 사료된다.

Keywords

References

  1. Wark, K. and Warner, C. F., 'Air pollution; Its origin and control,' Harper Collins, 2th Edition, pp. 1-5(1981)
  2. Cooper, D. C. and Alley, F. C., 'Air pollution control : A design approach,' Waveland Press, Inc., pp. 321 - 323(2002)
  3. Tsou, J., Pinard, L., Magnoux, P., Figueiredo, J. L., and Guisnet, M. 'Catalytic oxidation of volitale organic compounds(VOCs) Oxidation of o-xylene over Pt/HBEA catalysts,' Appl. Catal., B : Environ., 46, 371-379(2003) https://doi.org/10.1016/S0926-3373(03)00274-1
  4. Hodgson, J. W., Irick, D. K., and Fussell, L. M., 'Automotive engines and vehicles, in environmental analysis and remediation,' R. A. Meyersed. Johj Wiley & Sons, Inc., 552 - 572(1998)
  5. US Environmental Protection Agency, 'The clean air act amendments of 1990 : A guide for small business,' 450-K-92-001, pp. 1-27(1990)
  6. Noordally, E., Richmond, J. R., and Tahir, S. F., 'Destruction of volatile organic compounds by catalytic oxidation,' Catal. Today, 17, 359-366(1993) https://doi.org/10.1016/0920-5861(93)80039-4
  7. Luo, M. F., Yuan, X. X., and Zheng, X. M., 'Catalyst characterization and activity of Ag-Mn, Ag-Co and Ag-Ce composite oxide for oxidation of volatile organic compounds,' Appl. Catal., A: General, 175, 121-129 (1998) https://doi.org/10.1016/S0926-860X(98)00210-5
  8. Ferreia, R. S. G., Oliveira, P. G. P., and Noronha, F. B., 'Characterization and catalytic activity of $Pd/V_2O_5/A_2O_3$ catalysts on benzene total oxidation,' Appl. Catal., B: Environ., 50, 243-249(2004) https://doi.org/10.1016/j.apcatb.2004.01.006
  9. Janbey, A., Clark, W., Noordally, E., Grimes, S., and Tahir, S., 'Noble metal catalysts for methane removal,' Chemosphere, 52, 1041 - 1046(2003) https://doi.org/10.1016/S0045-6535(03)00292-3
  10. 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: General., 234, 65-78(2002) https://doi.org/10.1016/S0926-860X(02)00214-4
  11. Yim, S. D. and Nam, I. S., 'Characteristics of chromium oxides supported on $TiO_2$ and $Al_2O_3$ for the decomposition of perchloroethylene,' J. Catal., 221, 601-611 (2004) https://doi.org/10.1016/j.jcat.2003.09.026
  12. Park, P. W. and Ledford, J. S., 'The influence of surface structure on the catalytic activity of alumina supported copper oxide catalysts. Oxidation of carbon monoxide and methane,' Appl. Catal., B: Environ., 15, 221 -231(1998) https://doi.org/10.1016/S0926-3373(98)80008-8
  13. Lichtenberger, J. and Amiridis, M. D., 'Catalytic oxidation of chlorinated benzenes over $V_2O_5/TiO_2$ catalysts,' J. Catal., 223, 296-308(2004) https://doi.org/10.1016/j.jcat.2004.01.032
  14. Hong, S. S., Lee, G. H., and Lee, G. D., 'Catalytic combution of benzene over supported metal oxide catalysts,' Korean J. Chem. Eng., 20, 440-444(2003) https://doi.org/10.1007/BF02705544
  15. Einaga, H. and Futamura, S., 'Catalytic oxidation benzene with ozone over alumina-supported manganese oxides,' J. Catal., 227, 304-312(2004) https://doi.org/10.1016/j.jcat.2004.07.029
  16. Qi, G., Yang, R. T., and Chang, R., '$MnOx-CeO_2$ mixed oxides prepared by co-precipitation for selective catalytic reduction of NO with $NH_3$ at low temperatures,' Appl. Catal., B: Environ., 51, 93-106(2004) https://doi.org/10.1016/j.apcatb.2004.01.023
  17. Chang, Y. F. and McCarty, J. G., 'Novel oxygen storage components for advanced catalysts for emission control in natural gas fueled vehicles,' Catal. Today, 30, 163 - 170(1996) https://doi.org/10.1016/0920-5861(95)00007-0
  18. Stobbe, E. R., Boer, B. A., and Geus, J. W., 'The reduction and oxidation behaviour of manganese oxides,' Catal. Today, 47, 161-167(1999) https://doi.org/10.1016/S0920-5861(98)00296-X
  19. Silva, A. M. T., Marques, R R. N., and Quinta-Ferreira, R. M., 'Catalysts based in cerium oxide for wet oxidation of acrylie acid in the prevention of environmental risks,' Appl. Catal., B: Environ., 47, 269-279 (2004) https://doi.org/10.1016/j.apcatb.2003.09.019
  20. Alvarez-Galvan, M. C., O'Shea, V. A., Fierro, J. L. G., and Arias, P. L., 'Alumina-supported manganese and manganese-palladium oxide ,catalysts for VOCs combustion,' Catal. Communication, 4, 223 - 228(2003) https://doi.org/10.1016/S1566-7367(03)00037-2
  21. Qi, G. and Yang, R. T., 'Performance and kinetics study for low-temperature SCR of NO with $NH_3$ over MnOx-$CeO_2$, catalyst,' J. Catal., 217, 434-441(2003)
  22. Centeno, M. A., Paulis, M., Montes, M., and Oriozola, 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
  23. Ertl, G., Knozinger, H., and Weitkamp, J., 'Environmental catalysis,' WILEY-VCH, 39-40(1999)
  24. Salomonsson, P., Johansson, S., and Kasemo, B., 'Methane oxidation over pdox-on the mechanism for the hysteresis in activity and oxygen-content,' Catal. Lett., 33, 1-13(1995) https://doi.org/10.1007/BF00817041
  25. Lopez, E. F., Escribano, V. S., Resini, C., Amores, J. M. G., and Busca, G., 'A study of copreipitated Mn-Zr oxides and their behaviour as oxidation catalysts,' Appl. Catal., B: Environ., 29, 251-261(2001) https://doi.org/10.1016/S0926-3373(00)00206-X
  26. Spivey, J. J. and Butt, J. B., 'Literature Review: Deactivation of catalysts in the oxidation of volatile organic compounds,' Catal. Today, 11, 465 - 500(1992) https://doi.org/10.1016/0920-5861(92)80039-P
  27. Burch, R. and Loader, P. K., 'Investigation of $Pt/Al_2O_3$ and $Pd/Al_2O_3$ catalysts for the combustion of methane at low concentrations,' Appl. Catal., B: Environ., 5, 149-164(1994) https://doi.org/10.1016/0926-3373(94)00037-9
  28. Gangwal, S. K., Mullins, M. E., Spivey, J. J., and Caffrey, P. R., 'Kinetics and selectivity of deep catalytic oxidation of n-Hexane and benzene,' Appl. Catal., 36, 231-247(1988) https://doi.org/10.1016/S0166-9834(00)80118-9
  29. Alvarez-Galvan, M. C., Pawelec, B., de la Pena O'Shea, V. A., Fierro, J. L. G., and Arias, P. L., 'Formaldehyde/methanol combustion on alumina-supported manganesepalladium oxide catalyst,' Appl. Catal., B: Environ., 51, 79 - 87(2004) https://doi.org/10.1016/S0926-3373(04)00293-0