View PDF Version
 
DOI: 10.1039/A605341F (Paper) Reference Section for: J. Chem. Soc., Faraday Trans., 1997, 93, 175-180

FTIR studies on the selective oxidation and combustion of light hydrocarbons at metal oxide surfaces Part 3.—Comparison of the oxidation of C3 organic compounds over Co3O4, MgCr2O4 and CuO

(Note: The full text of this document is currently only available in the PDF Version )

Elisabetta Finocchio, Ronald J. Willey, Guido Busca and Vincenzo Lorenzelli

Abstract

Oxidation of the C3 organic compounds propane, propene, acrolein, propan-2-ol and acetone has been investigated over three transition-metal oxide catalysts, Co3O4, MgCr2O4 and CuO, in a flow reactor and using FTIR spectroscopy to study the adsorbed species. Co3O4 and MgCr2O4 are very active in propane and propene catalytic combustion. FTIR studies suggest that adsorbed isopropoxide species and adsorbed acetone and acetates are intermediates in propane oxidation while adsorbed acrolein and acrylates are intermediates in propene oxidation. Flow reactor studies support these hypotheses. It is suggested that the reaction rates in propane and propene total oxidation can be influenced, at low temperature, by the rate of oxidation of adsorbed acetate and acrylate intermediates, respectively. Co3O4 and MgCr2O4 are also active and quite selective catalysts for the oxy-dehydrogenation of propan-2-ol to acetone at low conversion, suggesting that the same oxygen species are involved in total and partial oxidation of organic compounds. CuO, as such, is not active in the adsorption and oxidation of C3 hydrocarbons and oxygenates, at low temperature. At higher temperatures the reactants reduce the catalyst and catalytic activity starts. The oxidation state of the CuOx catalyst can be evaluated by IR studying the transmittance of the radiation upon different treatments.

References

  1. Environmental Catalysis, ACS Symp. Ser. 552, ed. J. N. Armor, American Chemical Society, Washington DC, 1994 Search PubMed.
  2. J. J. Spivey, Ind. Eng. Chem. Res., 1987, 26, 2165 CrossRef CAS; J. J. Spivey, in Catalysis, The Royal Society of Chemistry, Cambridge, 1989, vol. 8, p. 158 Search PubMed.
  3. M. F. M. Zwinkels, S. G. Jaras, P. G. Menon and T. A. Griffin, Catal. Rev. Sci. Eng., 1993, 35, 319 Search PubMed.
  4. A. Bielanski and J. Haber, Oxygen in Catalysis, Dekker, New York, 1991 Search PubMed.
  5. P. Mars and D. W. van Krevelen, Chem. Eng. Sci, 1954, 3, 41 CAS.
  6. C. N. Satterfield, Heterogeneous Catalysis in Industrial Practice, McGraw Hill, New York, 2nd edn., 1991 Search PubMed.
  7. G. C. Bond, Heterogeneous catalysis, Principles and Applications, Oxford University Press, Oxford, 2nd edn., 1987 Search PubMed.
  8. J. E. Germain and R. Perez, Bull. Soc. Chim. Fr., 1972, 4683.
  9. G. K. Boreskov, in Catalysis Science and Technology, ed. J. R. Anderson and M. Boudart, Springer-Verlag, Berlin, 1985, vol. 3, p. 39 Search PubMed.
  10. J. E. Germain and L. Laugier, Bull. Soc. Chim. Fr., 1972, 541 and 2910 CAS.
  11. E. Garbowski, M. Guenin, M.-C. Marion and M. Primet, Appl. Catal., 1990, 64, 209 CrossRef CAS.
  12. L. Margolis, Adv. Catal., 1963, 14, 429 CAS.
  13. F. G. Dwyer, Catal. Rev. Sci. Eng., 1972, 6, 261 Search PubMed.
  14. E. Finocchio, G. Busca, V. Lorenzelli and R. J. Willey, J. Chem. Soc., Faraday Trans., 1994, 90, 3347 RSC.
  15. E. Finocchio, G. Busca, V. Lorenzelli and R. J. Willey, J. Catal., 1995, 151, 204 CrossRef CAS.
  16. E. Finocchio, G. Busca and V. Lorenzelli, J. Chem. Soc., Faraday Trans., 1996, 92, 1587 RSC.
  17. V. A. Kutznetsov, S. V. Gerei and Ya. B. Gorokhovatskii, Kinet. Katal., 1977, 18, 710 Search PubMed.
  18. A. A. Davydov, Infrared Spectroscopy of Adsorbed Species on the Surface of Transition Metal Oxides, Wiley, New York, 1990 Search PubMed.
  19. H. H. Voge and C. R. Adams, Adv. Catal. Relat. Subj., 1967, 17, 151 Search PubMed.
  20. A. Gil, P. Ruiz and B. Delmon, J. Catal., 1996, 159, 496 CrossRef CAS.
  21. J. C. Volta, P. Turlier and Y. Trambouze, J. Catal., 1974, 34, 329 CrossRef CAS.
  22. G. Busca, J. Mol. Catal., 1987, 43, 225 CrossRef CAS.
  23. K. NakamotoInfrared and Raman Spectra of Inorganic and Coordination Compounds, Wiley, New York, 4th edn., 1986, p. 232 Search PubMed.
  24. F. S. Stone, Bull. Soc. Chim. Fr., 1966, 819 CAS.
  25. J. Bloem, Phillips Rev. Rept., 1958, 13, 167 Search PubMed.
  26. G. Busca, E. Finocchio, G. Ramis and G. Ricchiardi, Catal. Today, in the press Search PubMed.
  27. A. Terlecki-Baricevic, B. Grbic, D. Jovanovic, S. Angelov, D. Mehandziev, C. Morinova and P. Kirilov-Stefanov, Appl. Catal., 1989, 47, 145 CrossRef CAS.
  28. K. R. Barnard, K. Foger, T. W. Tunney and R. D. Williams, J. Catal., 1990, 125, 265 CrossRef CAS.
  29. H. G. Lintz and K. Wittstock, Catal. Today, 1996, 29, 457 CrossRef CAS.
Click here to see how this site uses Cookies. View our privacy policy here.