Skip to main content
SpringerLink
Log in

Surface species in the direct amination of methanol over Brønsted acidic mordenite catalysts

  • Published:
Research on Chemical Intermediates Aims and scope Submit manuscript

Abstract

Quantitative in situ infrared spectroscopy in combination with kinetic analysis is utilized to derive mechanistic aspects for the reaction of methanol with ammonia on Brønsted acidic mordenite. Under non-reactive conditions, a coadsorption complex between methanol and ammonia is found, in which only ammonia is in direct interaction with the Brønsted acid sites of the zeolite. This complex is proposed to be the precursor for the formation of protonated methylamines in the zeolite pores which are formed in sequential order up to tetramethylammonium ions. These methylamines are unable to desorb under reaction conditions in the absence of ammonia. They leave the surface either by ammonia adsorption assisted desorption or by scavenging of methyl groups from protonated methylamines by ammonia. Both steps are concluded to be potentially rate determining.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

References

  1. L.D. Pesce and W.R. Jenks, in J.A. Kent (Ed.), Riegel's Handbook of Industrial Chemistry, 9th ed., Van Nostrand Reinold, New York, 1992, p. 1109.

    Google Scholar 

  2. M.G. Turcotte and T.A. Johnson, in J.I. Kroschwitz (Ed.), Kirk-Othmer Encyclopedia of Chemical Technology, 4th ed., John Wiley & Sons, New York, 1992, Vol. 2, p. 369.

    Google Scholar 

  3. L.A. Hamilton, US Patent 3.384.667, 1968.

  4. D.G. Parker and A.J. Tompsett, GB Patent 20119394B, 1982.

  5. F.J. Weigert, US Patent 4.313.003, 1982.

  6. M. Deeba and R.N. Chochran, Eur. Patent Appl. 85.408, 1983

  7. A.J. Tompsett, US Patent 4.436.938, 1984.

  8. Y. Ashina, M. Fujita, K. Niwa, and Y. Yagi, Eur. Patent Appl., 125.616, 1984.

  9. R.D. Shannon, M. Keane, Jr., L. Abrams, R.H. Staley, T.E. Gier, D.R. Corbin, and G.C. Sonnichsen, J. Catal., 113, 367 (1988).

    Article  CAS  Google Scholar 

  10. R.D. Shannon, M. Keane, Jr., L. Abrams, R.H. Staley, T.E. Gier, D.R. Corbin, and G.C. Sonnichsen, J. Catal., 114, 8 (1988).

    Article  CAS  Google Scholar 

  11. R.D. Shannon, M. Keane, Jr., R.H. Staley, T.E. Gier, and G.C. Sonnichsen, J. Catal., 115, 79 (1989).

    Article  CAS  Google Scholar 

  12. Y. Ashina, T. Fujita, M. Fukatsu, K. Niwa and Y. Yagi, Stud. Surf. Sci. Catal. 28, 779 (1986).

    Article  CAS  Google Scholar 

  13. K. Segawa and H. Tachibana, J. Catal, 131, 482 (1991).

    Article  CAS  Google Scholar 

  14. U. Dingerdissen, E. Nagy and F. Fetting, Chem.-Ing. Tech., 63, 625 (1991).

    Article  CAS  Google Scholar 

  15. A. Kogelbauer, Ch. Gründling, and J.A. Lercher, Stud. Surf. Sci. Catal., 84, 1475 (1994).

    Article  CAS  Google Scholar 

  16. I. Mochida, A. Yasutake, H. Fujitsu and K. Takeshita, J. Catal., 82, 313 (1983).

    Article  CAS  Google Scholar 

  17. M. Keane, Jr., G.C. Sonnichsen, L. Abrams, D.R. Corbin, T.E. Gier, and R.D. Shannon, Appl. Catal., 32, 361 (1987).

    Article  CAS  Google Scholar 

  18. L. Abrams, D.R. Corbin, and M. Keane, Jr., J. Catal., 126, 610 (1990).

    Article  CAS  Google Scholar 

  19. F. Fetting and U. Dingerdissen, Chem. Eng. Technol., 15, 202 (1992).

    Article  CAS  Google Scholar 

  20. F.J. Weigert, J. Catal., 103, 20 (1987).

    Article  CAS  Google Scholar 

  21. D.T. Chen, L. Zhang, J.M. Kobe, Chen Yi, and J.A. Dumesic, J. Molec. Catal., 93, 337 (1994).

    Article  CAS  Google Scholar 

  22. M. Sawa, M. Niwa, and Y. Murakami, Zeolites, 10, 532 (1990).

    Article  CAS  Google Scholar 

  23. G. Mirth, F. Eder and J.A. Lercher, J. Appl. Spectrosc., 48, 194 (1994).

    Article  CAS  Google Scholar 

  24. A. Kogelbauer, Ph.D. Thesis, TU Vienna, Austria, 1991.

  25. M.T. Aronson, R.J. Gorte, and W.E. Farneth, J. Catal., 105, 455 (1987).

    Article  CAS  Google Scholar 

  26. G. Mirth, J.A. Lercher, M.W. Anderson and J. Klinowski, J. Chem. Soc. Faraday Trans., 4, 702 (1988).

    Google Scholar 

  27. L. Kubelkova, J. Novakova, and K. Nedomova, J. Catal., 124, 441 (1990).

    Article  CAS  Google Scholar 

  28. G. Mirth, A. Kogelbauer, and J.A. Lercher, in R. van Ballmoos et al. (Eds.), Proc. 9th IZC, Butterworth-Heinemann, Montreal, 1992, p. 251.

    Google Scholar 

  29. L.H. Little, Infrared Spectra of Adsorbed Species, Academic Press, London, 1966, p. 180.

    Google Scholar 

  30. A. Kogelbauer, J.A. Lercher, K.H. Steinberg, F. Roessner, A. Soellner, R.V. Dmitriev, J. Chem. Soc. Faraday Trans., 88, 2283 (1992).

    Article  CAS  Google Scholar 

  31. M.M. Mortland, J.J. Fripiat, J. Chaussidon, and J. Uytterhoeven, J. Phys. Chem., 67, 248 (1963).

    Article  CAS  Google Scholar 

  32. E.H. Teunissen, R.A. van Santen, A.P.J. Jansen, and F.B. Duijneveldt, J. Phys. Chem., 97, 203 (1993).

    Article  CAS  Google Scholar 

  33. B. Chenon and C. Sandorfy, Can. J. Chem., 36, 1181 (1958).

    Article  CAS  Google Scholar 

  34. A.K. Ghosh and G. Curthoys, J. Chem. Soc. Faraday Trans. I, 80, 99 (1984).

    Article  CAS  Google Scholar 

  35. C. Brisette and C. Sandorfy, Can. J. Chem., 38, 34 (1960)

    Article  Google Scholar 

  36. E. Jobson, A. Baiker, and A. Wokaun, J. Chem. Soc. Faraday Trans., 86, 1131 (1990).

    Article  CAS  Google Scholar 

  37. A. Kogelbauer and J.A. Lercher, J. Chem. Soc. Faraday Trans., 88, 2283 (1992).

    Article  CAS  Google Scholar 

  38. A. Kogelbauer, Ch. Gründling, and J.A. Lercher, J. Phys. Chem., submitted for publication (1995).

  39. D.T. Chen, L. Zhang, Chen Yi and J.A. Dumesic, J. Catal., 146, 257 (1994).

    Article  CAS  Google Scholar 

  40. D.J. Parrillo, R.J. Gorte, and W.E. Farneth, J. Am. Chem. Soc., 115, 12441 (1993).

    Article  CAS  Google Scholar 

  41. Ch. Gründling, Ph. D. Thesis, University of Twente, the Netherlands, 1995.

Download references

Author information

Authors and Affiliations

  1. Department of Chemical Technology, University of Twente, P.O. Box 217, 7500 AE, Enschede, The Netherlands

    CH. Gründling, G. Eder-Mirth & J. A. Lercher

Authors
  1. CH. Gründling
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. G. Eder-Mirth
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. J. A. Lercher
    View author publications

    You can also search for this author in PubMed Google Scholar

Rights and permissions

Reprints and permissions

About this article

Cite this article

Gründling, C., Eder-Mirth, G. & Lercher, J.A. Surface species in the direct amination of methanol over Brønsted acidic mordenite catalysts. Res. Chem. Intermed. 23, 25–40 (1997). https://doi.org/10.1163/156856797X00367

Download citation

  • Received:

  • Accepted:

  • Issue Date:

  • DOI: https://doi.org/10.1163/156856797X00367

Keywords

Search

Navigation