Influence of solid-state transformation time on the nucleation and growth of silicalite 1 prepared from layered silicate

Abstract

The nucleation and crystal growth of silicalite 1 precursors synthesized by solid-state transformation were studied using X-ray diffraction, thermal analysis, IR spectroscopy,²⁹Si and ¹³C NMR and electron microscopy. Silicalite 1 was obtained after 16 h at 130 °C in a closed glass ampoule. Comparison with hydrothermal synthesis showed that the characterization of the precursors presents some similarities, however, nucleation and crystal growth were much shorter for solid-state transformation. ²⁹Si NMR showed that nucleation started during the first stage (cation exchange) for solid-state transformation, but only during the second stage for solid-state transformation. It was also observed that the major changes occurred during the beginning of crystal growth for solid-state transformation but during nucleation for hydrothermal synthesis. The results were explained by the fact that the starting materials were completely different: single layered silicate for solid-state transformation and colloidal silica for hydrothermal synthesis.

References

1. V. R. Choudhary and S. Mayadevi, Zeolites, 1996, 17, 501.
2. T. Sano, H. Yanagishita, Y. Kiyozumi, F. Mizukami and K. Haraya, J. Membr. Sci., 1994, 95, 221.
3. E. M. Flanigen, J. M. Bennett, R. W. Grose, J. P. Cohen, R. L. Patton, R. M. Kirchner and J. V. Smith, Nature (London), 1978, 271, 512.
4. S. L. Burkett and M. E. Davis, J. Phys. Chem., 1994, 98, 4647.
5. D. Tao, F. Fangxia, X. Yongzhuang and C. Jinghui, React. Kinet. Catal. Lett., 1997, 61, 97.
6. S. Shimizu, Y. Kiyozumi, K. Maeda, F. Mizukami, G. Pál-Borbély, R. M. Mihályi and H. Beyer, Adv. Mater., 1996, 8–9, 759.
7. G. Lagaly, Adv. Colloid Interface Sci., 1979, 11, 105.
8. E. G. Derouane, S. Detremmerie, Z. Gabelica and N. Blom, Appl. Catal., 1981, 1, 201.
9. K. F. M. G. J. Scholle, W. S. Veeman, P. Frenken and G. P. M. van der Velden, Appl. Catal., 1985, 17, 233.
10. C. D. Chang and A. T. Bell, Catal. Lett., 1991, 8, 305.
11. T. Yanagisawa, T. Shimizu, K. Kuroda and C. Kato, Bull. Chem. Soc. Jpn., 1990, 63, 988.
12. Z. Johan and G. F. Maglione, Bull. Soc. Minéral. Cristallogr., 1972, 95, 371.
13. S. Hayashi, J. Mater. Chem., 1997, 7, 1043.
14. B. M. Lok, T. R. Cannan and C. A. Messina, Zeolites, 1983, 3, 282.
15. G. Coudurier, C. Naccache and J. C. Vedrine, J. Chem. Soc., Chem. Commun., 1982, 1413.
16. P. A. Jacobs, E. G. Derouane and J. Weitkamp, J. Chem. Soc., Chem. Commun., 1981, 591.
17. G. Engelhardt and D. Michel, in High-Resolution Solid-State NMR of Silicates and Zeolites, John Wiley & Sons, Chichester, 1987, p. 129.
18. S. Inagaki, Y. Fukushima and K. Kuroda, Stud. Surf. Sci. Catal., 1994, 84, 125.