Advertisement

Journal of Materials Science

, Volume 37, Issue 10, pp 1959–1965 | Cite as

The synthesis and characterization of titanium silicalite-1

  • Y. G. Li
  • Y. M. Lee
  • J. F. Porter
Article

Abstract

This paper investigates the effect of the variation in alkoxide precursor ratio and templating agent concentration on the production of titanium silicalite (TS-1) through analysis using various physical characterisation techniques. X-ray diffraction showed clear evidence for the MFI zeolite structure and a high degree of crystallinity in all systems. For those materials prepared using a templating agent with ultra low alkali metal content, excellent agreement with previously reported unit cell parameters was obtained. For these same systems, 20% higher specific surface areas were also obtained by nitrogen adsorption. Analysis using an energy dispersive x-ray spectrometer coupled to a scanning electron microscope showed that the product typically contained between 60 and 90% of the titanium in the precursor and some dependence of titanium incorporation on the initial mixture composition was also observed. The results from Raman spectroscopy indicated titanium incorporation into the silicalite framework for all systems. For those materials produced using a templating agent with low alkali metal content, extra-framework anatase titanium dioxide was also identified at moderate Ti : Si mole ratios (>0.03) in the initial mixture. Due to its lower penetration depth, x-ray photoelectron spectroscopy (XPS) was used to characterise the titanium species in the surface layer. The XPS results indicated that a small amount of extra-framework titania was present in the surface of most of the TS-1 samples and the proportion of extra-framework material was observed to increase with both precursor alkali metal content and precursor titanium to silicon ratio.

Keywords

Silicalite Templating Agent Titanium Species Anatase Titanium Titanium Silicalite 
These keywords were added by machine and not by the authors. This process is experimental and the keywords may be updated as the learning algorithm improves.

Preview

Unable to display preview. Download preview PDF.

Unable to display preview. Download preview PDF.

REFERENCES

  1. 1.
    M. TARAMASSO, G. PEREGO and B. NOTARI, U.S. Patent 4,410,501 (1983).Google Scholar
  2. 2.
    A. ESPOSITO, C. NERI, F. BUONOMO and M. TARAMASSO, U.K. Patent 2,116,974B (1985).Google Scholar
  3. 3.
    P. ROFFIA, G. MANTEGAZZA, M. PADOVAN, G. PETRINI, S. TONTI and P. GERVASUTTI, Stud. Surf. Sci. Catal. 55 (1990) 43.Google Scholar
  4. 4.
    U. ROMANO, A. ESPOSITO, F. MASPERO, C. NERI and M. G. CLERICI, Stud. Surf. Sci. Catal. 55 (1990) 33.Google Scholar
  5. 5.
    M. G. CLERICI, Appl. Catal. 68 (1991) 249.Google Scholar
  6. 6.
    A. THANGARAJ, S. SIVASANKER and P. RATNASAMY, J. Catal. 131 (1991) 294.Google Scholar
  7. 7.
    A. J. H. P. VAN DER POL and J. H. C. VAN HOOFF, Appl. Catal. A 92 (1992) 93.Google Scholar
  8. 8.
    F. MASPERO and U. ROMANO, J. Catal. 146 (1994) 476.Google Scholar
  9. 9.
    A. THANGARAJ, M. J. EAPEN, S. SIVASANKER and P. RATNASAMY, Zeolites 12 (1992) 943.Google Scholar
  10. 10.
    R. MILLINI, E. PREVIDE MASSARA, G. PEREGO and G. BELLUSSI, J. Catal. 137 (1992) 497.Google Scholar
  11. 11.
    B. NOTARI, Stud. Surf. Sci. Catal. 37 (1988) 413.Google Scholar
  12. 12.
    C. B. KHOUW, C. B. DARTT, J. A. LABINGER and M. E. DAVIS, J. Catal. 149 (1994) 195.Google Scholar
  13. 13.
    G. PEREGO, G. BELLUSSI, C. CORDO, M. TARAMASSO, F. BUONOMO and A. ESPOSITO, Stud. Surf. Sci. Catal. 28 (1986) 129.Google Scholar
  14. 14.
    D. R. C. HUYBRECHTS, L. DE BRUYCKER and P. A. JACOBS, J. Mol. Catal. 71 (1992) 184.Google Scholar
  15. 15.
    G. DEO, A. M. TUREK, I. E. WACHS, D. R. C. HUYBRECHTS and P. A. JACOBS, Zeolites 13 (1993) 365.Google Scholar
  16. 16.
    M. G. CLERICI and P. INGALLINA, J. Catal. 140 (1993) 71.Google Scholar
  17. 17.
    A. THANGARAJ, R. KUMAR, S. P. MIRAJKAR and P. RATNASAMY, J. Catal. 130 (1991) 1.Google Scholar
  18. 18.
    M. A. CAMBLOR, A. CORMA and J. PEREZ-PARIENTE, Zeolites 13 (1993) 82.Google Scholar
  19. 19.
    G. BUSCA, G. RAMIS, J. M. GALLARDO AMORES, V. SANCHEZ ESCRIBANO and P. PIAGGIO, J. Chem. Soc. Faraday Trans. 90 (1994) 3181.Google Scholar
  20. 20.
    R. MILLINI, E. PREVIDE MASSARA, G. PEREGO and G. BELLUSSI, J. Catal. 68 (1992) 479.Google Scholar
  21. 21.
    D. TRONG ON, I. DENIS, C. LORTIE, C. CARTIER and L. BONNEVIOT, Stud. Surf. Sci. Catal. 83 (1994) 101.Google Scholar
  22. 22.
    P. BEHRENS, J. FELSCHE, S. VETTER, G. SCHULZELKOFF, N. I. JAEGER and W. NIEMANN, J. Chem. Soc. Chem. Commun. 10 (1991) 678.Google Scholar
  23. 23.
    G. N. VAYSSILOV, Catal. Rev.-Sci. Eng. 39(3) (1997) 209.Google Scholar
  24. 24.
    M. M. J. TREACY, J. B. HIGGINS and R. VON BALLMOOS, in “Collection of Simulated XRD Powder Diffraction Patterns for Zeolites”, third edition (revised). (1996) Elsevier, London.Google Scholar
  25. 25.
    A. TUEL and Y. BEN TAARIT, Zeolites 14 (1994) 272.Google Scholar
  26. 26.
    Idem., Applied Catalysis A 110 (1994) 137.Google Scholar
  27. 27.
    G. BELLUSSI and V. FATTORE, Stud. Surf. Sci. Catal. 69 (1991) 79.Google Scholar
  28. 28.
    S. VETTER, G. SCHULZ-EKLOFF, K. KULAWIK and N. I. JAEGER, Chem. Eng. Technol. 17 (1994) 348.Google Scholar
  29. 29.
    B. KRAUSHAAR, Ph.D. Thesis, Eindhoven University of Technology, 1989.Google Scholar
  30. 30.
    R. VON BALLMOOS and W. M. MEIER, Nature 389 (1981) 782.Google Scholar
  31. 31.
    G. ZHANG, J. STERTE and B. J. SCHOEMAN, Chem. Mater. 9 (1997) 210.Google Scholar
  32. 32.
    R. J. DAVIS, Z. LIU, J. E. TABORA and W. S. WIELAND, Catal. Lett. 34 (1995) 101.Google Scholar
  33. 33.
    E. ASTORINO, J. B. PERI, R. J. WILLEY and G. BUSCA, J. Catal. 157 (1995) 482.Google Scholar
  34. 34.
    A. ZECCHINA, G. SPOTO, S. BORDIGA, A. FERRERO, G. PETRINI, G. LEOFANTI and M. PADOVAN, Stud. Surf. Sci. Catal. 69 (1991) 251.Google Scholar
  35. 35.
    E. DUPREY, P. BEAUNIER, M.-A. SPRINGUEL-HUET, F. BOZON-VERDURAZ, J. FRAISSARD, J.-M. MANOLI and J.-M. BREGEAULT, J. Catal. 165 (1997) 22.Google Scholar
  36. 36.
    Y.-H. ZHANG, C. K. CHAN, J. F. PORTER and W. GUO, J. Mater. Res. 13(9) (1998) 2602.Google Scholar
  37. 37.
    M. TARAMASSO, G. MANARA, V. FATTORE and B. NOTARI, U.S. Patent 4,666,692 (1987).Google Scholar
  38. 38.
    G. BELLUSSI, A. CARATI, M. G. CLERICI and A. ESPOSITO, Stud. Surf. Sci. Catal. 63 (1991) 421.Google Scholar
  39. 39.
    S. M. MUKHOPAHYAY and S. H. GAROFALINI, J. Non-Crystal. Solids 126 (1990) 202.Google Scholar
  40. 40.
    A. Y. STAKHEEV, E. S. SHPIRO and J. APIJOK, J. Phys. Chem. 97 (1993) 5668.Google Scholar
  41. 41.
    D. TRONG ON, L. BONNEVIOT, A. BITTAR, A. SAYARI and S. KALIAGUINE, J. Mol. Catal. 74 (1992) 233.Google Scholar

Copyright information

© Kluwer Academic Publishers 2002

Authors and Affiliations

  • Y. G. Li
    • 1
  • Y. M. Lee
    • 1
  • J. F. Porter
    • 1
  1. 1.Department of Chemical EngineeringHong Kong University of Science & TechnologyHong Kong SAR, People's Republic of China

Personalised recommendations