Skip to main content
SpringerLink
Log in

In situ NMR spectroscopy in heterogeneous catalysis: Kinetic study of hydrocarbon conversion mechanisms

  • Mechanisms of Catalytic Reactions
  • Published:
Kinetics and Catalysis Aims and scope Submit manuscript

Abstract

The potential of high-resolution solid-state NMR spectroscopy for kinetic and mechanistic studies of hydrocarbon conversion on solid acid catalysis between 20 and 300°C is considered. The use of this technique is illustrated by the elucidation of the mechanisms of hydrogen exchange and 13C label transfer in alkanes and olefins, n-butane isomerization on sulfated zirconia, and ethane aromatization on zinc-containing zeolite beta. The kinetic parameters determined in these studies provide a basis for quantum chemical calculations of possible hydrocarbon activation and conversion pathways and for evaluating the reliability and accuracy of these theoretical calculations.

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. Derouane, E.G., Gilson, J.-P., and Nagy, J.B., Zeolites, 1982, vol. 2, no. 1, p. 42.

    Article  CAS  Google Scholar 

  2. Van den Berg, J.P., Wolthuizen, J.P., Clague, A.D.H., Hays, G.R., Huis, R., and van Hoof, J.H.C., J. Catal., 1983, vol. 80, no. 1, p. 130.

    Article  Google Scholar 

  3. Anderson, M.W. and Klinowski, J., Nature, 1989, vol. 339, no, 6221, p. 200.

    Article  CAS  Google Scholar 

  4. Haw, J.F., Richardson, B.R., Oshio, I.S., Lazo, N.D., and Speed, J.A., J. Am. Chem. Soc., 1989, vol. 111, no. 6, p. 2052.

    Article  CAS  Google Scholar 

  5. Bosacek, V., J. Phys. Chem., 1993, vol. 97, no. 41, p. 10732.

    Article  CAS  Google Scholar 

  6. Murray, D.K., Chang, J.W., and Haw, J.F., J. Am. Chem. Soc., 1993, vol. 115, no. 11, p. 4732.

    Article  CAS  Google Scholar 

  7. Wang, W., Jiao, J., Jiang, Y.J., Ray, S.S., and Hunger, M., ChemPhysChem, 2005, vol. 6, no. 8, p. 1467.

    Article  CAS  Google Scholar 

  8. Stepanov, A.G., Romannikov, V.N., and Zamaraev, K.I., Catal. Lett., 1992, vol. 13, no. 4, p. 395.

    Article  CAS  Google Scholar 

  9. Stepanov, A.G., Zamaraev, K.I., and Thomas, J.M., Catal. Lett., 1992, vol. 13, no. 4, p. 407.

    Article  CAS  Google Scholar 

  10. Oliver, F.G., Munson, E.J., and Haw, J.F., J. Phys. Chem., 1992, vol. 96, no. 20, p. 8106.

    Article  CAS  Google Scholar 

  11. Goguen, P.W., Xu, T., Barich, D.H., Skloss, T.W., Song, W., Wang, Z., Nicholas, J.B., and Haw, J.F., J. Am. Chem. Soc., 1998, vol. 120, no. 11, p. 2650.

    Article  CAS  Google Scholar 

  12. Stepanov, A.G., Sidelnikov, V.N., and Zamaraev, K.I., Chem. Eur. J., 1996, vol. 2, no. 2, p. 157.

    Article  CAS  Google Scholar 

  13. Luzgin, M.V., Stepanov, A.G., Shmachkova, V.P., and Kotsarenko, N.S., J. Catal., 2001, vol. 203, no. 2, p. 273.

    Article  CAS  Google Scholar 

  14. Luzgin, M.V., Romannikov, V.N., Stepanov, A.G., and Zamaraev, K.I., J. Am. Chem. Soc., 1996, vol. 118, no. 44, p. 10 890.

  15. Luzgin, M.V. and Stepanov, A.G., Mendeleev Commun., 1996, vol. 6, no. 6, p. 238.

    Article  Google Scholar 

  16. Stepanov, A.G. and Luzgin, M.V., Chem. Eur. J., 1997, vol. 3, no. 1, p. 47.

    Article  CAS  Google Scholar 

  17. Derouane, E.G., Hamid, S.B.A., Ivanova, I.I., Blom, N., and Hojlund-Nielsen, P.E., J. Mol. Catal., 1994, vol. 86, nos. 1–3, p. 371.

    CAS  Google Scholar 

  18. Stepanov, A.G., Catal. Today, 1995, vol. 24, no. 3, p. 341.

    Article  CAS  Google Scholar 

  19. Stepanov, A.G., Luzgin, M.V., Arzumanov, S.S., Ernst, H., and Freude, D., J. Catal., 2002, vol. 211, no. 1, p. 165.

    CAS  Google Scholar 

  20. Luzgin, M.V., Arzumanov, S.S., Shmachkova, V.P., Kotsarenko, N.S., Rogov, V.A., and Stepanov, A.G., J. Catal., 2003, vol. 220, no. 1, p. 233.

    Article  CAS  Google Scholar 

  21. Luzgin, M.V., Stepanov, A.G., Arzumanov, S.S., Rogov, V.A., Parmon, V.N., Wang, W., Hunger, M., and Freude, D., Chem. Eur. J., 2006, vol. 12, no. 2, p. 457.

    Article  Google Scholar 

  22. Ipatieff, V.N. and Pines, H., J. Org. Chem., 1936, vol. 1, no. 5, p. 464.

    Article  CAS  Google Scholar 

  23. Stepanov, A.G., Ernst, H., and Freude, D., Catal. Lett., 1998, vol. 54, nos. 1–2, p. 1.

    Article  CAS  Google Scholar 

  24. Blaszkowski, S.R., Nascimento, M.A.C., and van Santen, R.A., J. Phys. Chem., 1996, vol. 100, no. 9, p. 3463.

    Article  CAS  Google Scholar 

  25. Haouas, M., Walspurger, S., Taulelle, F., and Sommer, J., J. Am. Chem. Soc., 2004, vol. 126, p. 599.

    Article  CAS  Google Scholar 

  26. Haouas, M., Walspurger, S., and Sommer, J., J. Catal., 2003, vol. 215, no. 1, p. 122.

    Article  CAS  Google Scholar 

  27. Stepanov, A.G., Arzumanov, S.S., Ernst, H., and Freude, D., Chem. Phys. Lett., 2006, vol. 420, nos. 4–6, p. 574.

    Article  CAS  Google Scholar 

  28. Stepanov, A.G., Arzumanov, S.S., Luzgin, M.V., Ernst, H., Freude, D., and Parmon, V.N., J. Catal., 2005, vol. 235, no. 1, p. 221.

    Article  CAS  Google Scholar 

  29. Arzumanov, S.S., Reshetnikov, S.I., Stepanov, A.G., Parmon, V.N., and Freude, D., J. Phys. Chem. B, 2005, vol. 109, no. 42, p. 19 748.

  30. Saunders, M., Hewett, A.P., and Kronja, O., Croat. Chim. Acta, 1992, vol. 65, no. 3, p. 673.

    CAS  Google Scholar 

  31. Stepanov, A.G., Arzumanov, S.S., Luzgin, M.V., Ernst, H., and Freude, D., J. Catal., 2005, vol. 229, no. 1, p. 243.

    Article  CAS  Google Scholar 

  32. Teraishi, K., J. Mol. Catal. A: Chem., 1998, vol. 132, no. 1, p. 73.

    Article  CAS  Google Scholar 

  33. Boronat, M., Viruela, P.M., and Corma, A., J. Am. Chem. Soc., 2004, vol. 126, no. 10, p. 3300.

    Article  CAS  Google Scholar 

  34. Saunders, M., Hagen, E.L., and Rosenfeld, J., J. Am. Chem. Soc., 1968, vol. 90, no. 24, p. 6882.

    Article  CAS  Google Scholar 

  35. Matsuhashi, H., Shibata, H., Nakamura, H., and Arata, K., Appl. Catal., A, 1999, vol. 187, no. 1, p. 99.

    Article  CAS  Google Scholar 

  36. Stepanov, A.G., Luzgin, M.V., Arzumanov, S.S., Wang, W., Hunger, M., and Freude, D., Catal. Lett., 2005, vol. 101, nos. 3–4, p. 181.

    Article  CAS  Google Scholar 

  37. Ono, Y., Catal. Rev. Sci. Eng., 1992, vol. 34, no. 3, p. 179.

    Article  CAS  Google Scholar 

  38. Biscardi, J.A., Meitzner, G.D., and Iglesia, E., J. Catal., 1998, vol. 179, no. 1, p. 192.

    Article  CAS  Google Scholar 

  39. Biscardi, J.A. and Iglesia, E., J. Catal., 1999, vol. 182, no. 1, p. 117.

    Article  CAS  Google Scholar 

  40. Hagen, A. and Roessner, F., Catal. Rev. Sci. Eng., 2000, vol. 42, no. 4, p. 403.

    Article  CAS  Google Scholar 

  41. Kazansky, V.B., Serykh, A.I., and Pidko, E.A., J. Catal., 2004, vol. 225.

  42. Kazansky, V.B. and Pidko, E.A., J. Phys. Chem. B, 2005, vol. 109, no. 6, p. 2103.

    Article  CAS  Google Scholar 

  43. Kazansky, V.B., Subbotina, I.R., Rane, N., van Santen, R.A., and Hensen, E.J.M., Phys. Chem. Chem. Phys., 2005, vol. 7, no. 16, p. 3088.

    Article  CAS  Google Scholar 

  44. Larson, J.G. and Hall, W.K., J. Phys. Chem., 1965, vol. 69, no. 9, p. 3080.

    Article  CAS  Google Scholar 

  45. Lee, B., Kondo, J.N., Wakabayashi, F., and Domen, K., Catal. Lett., 1999, vol. 59, no. 1, p. 51.

    Article  CAS  Google Scholar 

  46. Schoofs, B., Martens, J.A., and Schoonheydt, R.A., J. Catal., 1999, vol. 183, no. 2, p. 355.

    Article  CAS  Google Scholar 

  47. Blaszkowski, S.R., Jansen, A.P.J., Nascimento, M.A.C., and van Santen, R.A., J. Phys. Chem., 1994, vol. 98, no. 49, p. 12 938.

  48. Zheng, X. and Blowers, P., J. Mol. Catal. A: Chem., 2005, vol. 242, no. 1, p. 18.

    Article  CAS  Google Scholar 

  49. Zheng, X. and Blowers, P., J. Mol. Catal. A: Chem., 2006, vol. 246, nos. 1–2, p. 1.

    Article  CAS  Google Scholar 

  50. Frash, M.V. and van Santen, R.A., Phys. Chem. Chem. Phys., 2000, vol. 2, no. 5, p. 1085.

    Article  CAS  Google Scholar 

  51. Zhidomirov, G.M., Shubin, A.A., Kazansky, V.B., and van Santen, R.A., Theor. Chem. Acc., 2005, vol. 114, nos. 1–3, p. 90.

    Article  CAS  Google Scholar 

  52. Kolyagin, Y.G., Ordomsky, V.V., Khimyak, Y.Z., Rebrov, A.I., Fajula, F., and Ivanova, I.I., J. Catal., 2006, vol. 238, no. 1, p. 122.

    Article  CAS  Google Scholar 

Download references

Author information

Authors and Affiliations

  1. Boreskov Institute of Catalysis, Siberian Branch, Russian Academy of Sciences, Novosibirsk, 630090, Russia

    A. G. Stepanov & V. N. Parmon

  2. Department of Surface Physics, University of Leipzig, Leipzig, Germany

    D. Freude

Authors
  1. A. G. Stepanov
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. V. N. Parmon
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. D. Freude
    View author publications

    You can also search for this author in PubMed Google Scholar

Additional information

Original Russian Text © A.G. Stepanov, V.N. Parmon, D. Freude, 2007, published in Kinetika i Kataliz, 2007, Vol. 48, No. 4, pp. 554–569.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Stepanov, A.G., Parmon, V.N. & Freude, D. In situ NMR spectroscopy in heterogeneous catalysis: Kinetic study of hydrocarbon conversion mechanisms. Kinet Catal 48, 521–534 (2007). https://doi.org/10.1134/S0023158407040088

Download citation

  • Received:

  • Issue Date:

  • DOI: https://doi.org/10.1134/S0023158407040088

Keywords

Search

Navigation