Journal of the Korean Applied Science and Technology (한국응용과학기술학회지)

The Korean Society of Applied Science and Technology (한국응용과학기술학회)
권호 표지
DOI QR코드

DOI QR Code

Synthesis of Methanol and Formaldehyde by Partial Oxidation of Methane over Mixed Oxide Catalysts

복합산화물 촉매 상에서 메탄의 부분산화에 의한 메탄올 및 포름알데히드의 합성

  • 함현식 (명지대학교 공과대학 화학공학과) ;
  • 신기석 (명지대학교 공과대학 화학공학과) ;
  • 안성환 (명지대학교 공과대학 화학공학과) ;
  • 김송형 (명지대학교 공과대학 화학공학과) ;
  • 홍석영 ;
  • 박홍수 (명지대학교 공과대학 화학공학과)
  • Published : 2006.09.30
Download PDF
⟨ Previous Next ⟩

Abstract

Methanol and formaldehyde were produced directly by the partial oxidation of methane over mixed oxide catalysts. The catalysts were composed of Mo and Bi with late-transition metals, such as Mn, Fe, and Co. The reaction was carried out at $450^{\circ}C$, 50 bar in a fixed-bed differential reactor. The prepared catalysts were characterized by $O_2-TPD$ and BET apparatus. Among the catalysts used, the catalyst composed of 1:1:2.5 molar ratio of Mo:Bi:Mn showed the best methane conversion and methanol selectivity. The change in ratio of methane to oxygen affected at the conversion and selectivity, and the most proper ratio was 10:1.5. Methane conversion, methanol and formaldehyde selectivities increased with the surface areas of the catalysts. From the $O_2-TPD$ result, it was found that the oxygen species responsible for this reaction might be the lattice oxygen species desorbed at high temperature around $800^{\circ}C$.

Keywords

References

  1. J. G. Michael and N. W. Green, Economic of Natural Gas Conversion Processes, Fuel Processing Technology, 42, 65(1995) https://doi.org/10.1016/0378-3820(94)00094-A
  2. R. Pitchai and K. Klier, Partial Oxidation of Methane, Catal. Rev. Sci. Eng. 28, 13(1986) https://doi.org/10.1080/03602458608068085
  3. S. H. Taylor, J. S. Hargreaves, G. J. Hutchings, and R. W. Toyner, Methane and Alkane Conversion Chemistry, Plenum, 339(1995)
  4. E. W. James, D. Mahajan, and G. Michael, Catalytic Route to Transport Fuels Utilizing Natural Gas Hydrates, Catalysis Today, 50, 97(1999) https://doi.org/10.1016/S0920-5861(98)00466-0
  5. K. Aoki, M. Ohmae, T. Nanba, K. Takeishi, N. Azuma, A. Ueno, H. Ohfune, H. Hayashi, and Y. Udagawa, Direct Conversion of Methane into Methanol over $MoO_3/SiO_2$ Catalyst in an Excess Amount of Water Vapor, Catalysis Today, 45, 29(1998) https://doi.org/10.1016/S0920-5861(98)00236-3
  6. H. F. Liu, R. S. Liu, K. Y. Liew, R. E. Johnson, and J. H. Lunsford, Partial Oxidation of Methane by Nitrous Oxide over Molybdenum on Silica, Journal of the American Chemical Society, 106, 15(1984)
  7. A. Erdohelyi, K. Fodor, R. Nemeth, A. Hancz, and A. Oszko, Partial Oxidation of Methane on Silica-Supported Different Alkali metal Molybdates, Journal of Catalysis, 199, 328(2001) https://doi.org/10.1006/jcat.2001.3178
  8. A. Franscesco, G. Nicola, and P. Adoflo, Working Mechanism of Oxide Catalysts in the Partial Oxiation of Mthane to Foramldehyde, Journal of Catalysis, 167, 66(1997) https://doi.org/10.1006/jcat.1997.1546
  9. M. Xu, M. P. Rosynek, and J. H. Lunsford, Reactions of Methyl Radicals with Metal Oxides, Preprints-American Chemical Society, 39(2), 283(1994)
  10. D. J. Thomas, R. Willi, and A. Baiker, Partial Oxidation of Methane: the Role of Surface Reactions, Ind Eng. Chemical. Reserch. 31, 2272(1992) https://doi.org/10.1021/ie00010a003
  11. K. Suzuki, T. Hayakawa, M. Shimizu, and K. Takehira, Partial Oxidation of Methane over Silica Supported Molybdeum oxide Catalysts, Catalyst Letters, 30, 15(1995)
  12. A. Erdohelyi, K. Fodor, and F. Solymosi, Partial Oxidation of Methane on Supported Potassium Molybdate, Journal of Catalysis, 166, 244(1997) https://doi.org/10.1006/jcat.1997.1519
  13. A. G. Gayubo and J. M. ortega, MTG Fluidized Bed Reactor-Regenerator Unit with Catalyst Circulation: Process Simulation and Operation of an Experimental Setup, Chemical Engineering Science, 55 3232(2000)
  14. K. Yoshizawa, Y. Shiota, and T. Yamabe, Methne to Methanol Conversion by $MnO^+$, $FeO^+$, $CoO^+$: A Theoretical Study of Catalytic Selectivy, Journal of American Chemical Society, 120, 564(1998) https://doi.org/10.1021/ja971723u
  15. K, Otsuka and K. Takayuki, Active Catalysts in Oxidative Coupling of Methane, Journal of the Chemical Society, Chemical Communications, 388(1987)
  16. Y. H. Han, W. Ueda, and M. O. Yoshihiko, Lattice Oxide Ion-Transfer Effect Demonstrated in the Selective Oxidation of Propane over Silica-Supported Bismuth Molybdate Catalysts, Applied Catalysis A: General, 176, 11(1999) https://doi.org/10.1016/S0926-860X(98)00204-X