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13C MAS NMR mechanistic study of the initial stages of propane activation over H-ZSM-5 zeolite

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Abstract

13C MAS NMR study of the early stages of propane 2-13C activation was performed over H-ZSM-5 catalysts with various content of protonic and aprotonic sites. The reaction mechanism was tested by addition of various probe-molecules (C3H6, C6H6, H2, H2O and CO). The results on tracing the fate of 13C label during this experiments conclude to a monofunctional mechanism involving propane protonation on the strong Brønsted sites of H-ZSM-5 and the formation of carbonium ion type transition states, which further evolve in four different ways leading to 13C scrambling in propane, cracking, dehydrogenation and disproportionation.

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References

  1. M. Guisnet, N.S. Gnep and F. Alario, Appl. Catal. 89 (1992) 1.

    Article  CAS  Google Scholar 

  2. Y. Ono, Catal. Rev. Sci. Eng. 34 (1992) 179.

    CAS  Google Scholar 

  3. B.W. Wojciechowski and A. Corma, Catalytic Cracking: Catalysts, Chemistry and Kinetics(Dekker, New York, 1986).

    Google Scholar 

  4. A. Brenner and P.H. Emmet, J. Catal. 75 (1982) 410.

    Article  CAS  Google Scholar 

  5. W.O. Haag and R.M. Dessau, in: Proc.8th Int.Congress on Catalysis(Verlag Chimie, Weinheim, 1984) p. 305.

    Google Scholar 

  6. H. Krannila, W.O. Haag and B.C. Gates, J. Catal. 135 (1992) 115.

    Article  CAS  Google Scholar 

  7. J. Abbot, J. Catal. 126 (1990) 628.

    Article  CAS  Google Scholar 

  8. J. Abbot, Appl. Catal. 57 (1990) 105.

    Article  CAS  Google Scholar 

  9. J. Engelhardt and W.K. Hall, J. Catal. 125 (1990) 472.

    Article  CAS  Google Scholar 

  10. T.F. Narbeshuber, H. Vinek and J.A. Lercher, J. Catal. 157 (1995) 388.

    Article  CAS  Google Scholar 

  11. G.K. Surya Prakash, ACS Symp. Ser. 571 (1994) 1.

    Google Scholar 

  12. G.B. McVicker, G.M. Kramer and J.J. Ziemiak, J. Catal. 92 (1985) 355.

    Article  Google Scholar 

  13. G.B. McVicker, G.M. Kramer and J.J. Ziemiak, J. Catal. 83 (1983) 286.

    Article  CAS  Google Scholar 

  14. R.A. Beyerlein, G.B. McVicker, L.M. Yacullo and J.J. Ziemiak, J. Phys. Chem. 92 (1988) 1967.

    Article  CAS  Google Scholar 

  15. T. Mole, J.R. Anderson and G. Creer, Appl. Catal. 17 (1985)141.

    Article  CAS  Google Scholar 

  16. M.V. Vishnetskaya and B.V. Romanowsky, J. Phys. Chem. (Rus.) 67 (1993) 1740.

    CAS  Google Scholar 

  17. H.G. Karge, in: Introduction to Zeolite Science and Practice, eds. H. van Bekkum, E.M. Flanigen and J.C. Jansen (Elsevier, Amsterdam, 1991) p. 531.

    Google Scholar 

  18. M.V. Anderson and J. Klinowski, Nature 339 (1989) 200.

    Article  CAS  Google Scholar 

  19. J.F. Haw, Spec. Publ.-R. Soc. Chem. 114 (1992) 133.

    Google Scholar 

  20. I.I. Ivanova and E.G. Derouane, Stud. Surf. Sci. Catal. 85 (1994) 357.

    CAS  Google Scholar 

  21. A.G. Stepanov, Catalysis Today 24 (1995) 341.

    Article  CAS  Google Scholar 

  22. E.G. Derouane, S.B. Abdul Hamid, I.I. Ivanova, N. Blom and P.E. Højlund-Nielsen, J. Mol. Catal. 86 (1994) 371.

    Article  CAS  Google Scholar 

  23. I.I. Ivanova, N. Blom, S.B. Abdul Hamid and E.G. Derouane, Recl. Trav. Chim. Pays-Bas 113 (1994) 454.

    CAS  Google Scholar 

  24. I.I. Ivanova, N. Blom and E.G. Derouane, Stud. Surf. Sci. Catal. 94 (1995) 419.

    Article  CAS  Google Scholar 

  25. I.I. Ivanova, N. Blom and E.G. Derouane, J. Mol. Catal. 109 (1996) 157.

    Article  CAS  Google Scholar 

  26. I.I. Ivanova and F. Fajula, in: 11th Intern.Zeolite Conf., Book of Abstracts, Seoul, August 12–17, 1996, p. RP64.

    Google Scholar 

  27. Z. Gabelica, E.G. Derouane and N. Blom, ACS Symp. Ser. 248 (1984) 219.

    Article  CAS  Google Scholar 

  28. M.I. Loktev and A.A. Slinkin, Uspekhi Khimii 45 (1976) 1594.

    CAS  Google Scholar 

  29. A. Lombardo and W.K. Hall, J. Catal. 112 (1988) 565.

    Article  CAS  Google Scholar 

  30. W.K. Hall, E.A. Lombardo and J.J. Engelhardt, J. Catal. 115 (1989) 611.

    Article  CAS  Google Scholar 

  31. A.E. Hirschler, J. Catal. 5 (1966) 196.

    Article  CAS  Google Scholar 

  32. G.A. Olah, J. Amer. Chem. Soc. 94 (1972) 808.

    Article  CAS  Google Scholar 

  33. M. Sanders, A.P. Hewett and O. Kronja, Croat. Chem. Acta. 65 (1992) 673.

    Google Scholar 

  34. G.A. Olah and A.M. White, J. Amer. Chem. Soc. 91 (1969) 5801.

    Article  CAS  Google Scholar 

  35. J.F. Haw, B.R. Richardson, I.S. Oshiro, N.D. Lazo and J.A. Speed, J. Am. Chem. Soc. 111 (1989) 2052.

    Article  CAS  Google Scholar 

  36. J.L. White, N.D. Lazo, B.R. Richardson and J.F. Haw, J. Catal. 125 (1990) 260.

    Article  CAS  Google Scholar 

  37. E.A. Lombardo, G.A. Sill and W.K. Hall, J. Catal. 119 (1989) 426.

    Article  CAS  Google Scholar 

  38. F. Fajula, Stud. Surf. Sci. Catal. 20 (1985) 361.

    Article  CAS  Google Scholar 

  39. M. Daage and F. Fajula, J. Catal. 81 (1983) 394.

    Article  CAS  Google Scholar 

  40. P.O. Fritz and J.H. Lunsford, J. Catal. 118 (1989) 85.

    Article  CAS  Google Scholar 

  41. R.M. Lago, W.O. Haag, R.J. Mikowsky, D.H. Olson, S.D. Hellring, K.D. Schmitt and G.T. Kerr, in: Proc.7th Int.Zeol.Conf., eds. Y. Murakami et al. (Kodansha, Tokyo, 1987) p. 677.

    Google Scholar 

  42. N.-Y. Tøpsoe, F. Joensen and E.G. Derouane, J. Catal. 110 (1984) 404.

    Article  Google Scholar 

  43. D.B. Lukianov, Zeolites 11 (1991) 325.

    Article  Google Scholar 

  44. G. Engelhardt and D. Michel, High-Resolution Solid-State NMR of Silicates and Zeolites(Wiley, Chichester, 1987) p. 379.

    Google Scholar 

  45. A. Michael, W. Meiler, D. Michel, H. Pfeifer, D. Hoppach and J. Delmau, J. Chem. Soc. Faraday Trans. 1 82 (1986) 3053.

    Article  CAS  Google Scholar 

  46. J.A. Lercher, R.A. van Santen and H. Vinek, Catalysis Letters 27 (1994) 91.

    Article  CAS  Google Scholar 

  47. E. Breitmaier, and W. Voelter, Carbon-13 NMR Spectroscopy(VCH, Weinheim, 1987).

    Google Scholar 

  48. J.B. Nagy, G. Engelgart and D. Michel, Adv. Colloid Interface Sci. 23 (1985) 67.

    Article  CAS  Google Scholar 

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Authors and Affiliations

  1. Department of Chemistry, Moscow State University, Vorobievy Gory, 119899, Moscow, Russia

    Irina I. Ivanova & Elena B. Pomakhina

  2. RAS, Institute of Petrochemical Synthesis, Leninsky pr. 29, 117012, Moscow, Russia

    Elena B. Pomakhina & Alexander I. Rebrov

  3. The University of Liverpool, The Leverhulme Centre for Innovative Catalysis, PO Box 147, Liverpool, L69 3BX, UK

    Eric G. Derouane

Authors
  1. Irina I. Ivanova
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  2. Elena B. Pomakhina
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  3. Alexander I. Rebrov
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  4. Eric G. Derouane
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Ivanova, I.I., Pomakhina, E.B., Rebrov, A.I. et al. 13C MAS NMR mechanistic study of the initial stages of propane activation over H-ZSM-5 zeolite. Topics in Catalysis 6, 49–59 (1998). https://doi.org/10.1023/A:1019139111671

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