Dielectric properties of an NaX zeolite as a function of the hydration state

Abstract

The dielectric properties of the NaX zeolite (Si/Al=1.3) have been measured after different thermal treatments in the temperature range 100–400°C. The frequency domain was varied from 10 to 10⁶ Hz, the measuring temperature being in the range 80–150°C. Independent of the outgassing temperature (i.e. the number of water molecules), the ac conductivity is ascribed to migration of the supercage cations. The variation in the migration energy (E_dc) as a function of the adsorbed water molecules (0.9–0.58 eV) shows their influence on the conduction process. Two relaxation domains are observed: ‘low-frequency’ and ‘high frequency’ relaxations, which are due to local hops of cations located in sites II and III, respectively. These two relaxations are confirmed by thermally stimulated current measurements. The energies associated with these relaxations vary with the outgassing temperature.

References

1. J. M. Thomas, in Zeolites: Facts, Figures, Future, ed. P. A. Jacobs and R. A. Van Santen, Elsevier, Amsterdam, 1989, p. 3.
2. G. A. Ozin, A. Kuperman and A. Stein, Angew. Chem., 1989, 101, 373.
3. W. M. Meier, D. H. Olson and C. Baerlocker, in Atlas of Zeolite Structures Types, Elsevier, London, 1996, p. 104.
4. W. J. Mortier, Compilation of Extra-framework Sites in Zeolites, Butterworth, Guilford, 1982, p. 19.
5. A. Chapton, G. Ravalitera, M. Choquet, B. Vandorpe and L. Gengembre, Rev. Phys. Appl., 1975, 10, 153.
6. P. Tabourier, J. C. Carru and W. Wacrenier, J. Chim. Phys., 1990, 87, 43.
7. J. J. Van Dun and W. J. Mortier, J. Phys. Chem., 1988, 92, 6740.
8. J. J. Van Dun, K. Dhaeze, W. J. Mortier and D. E. W. Vaughan, J. Phys. Chem. Solids, 1989, 50, 469.
9. O. Vigil, J. Fundora, F. Leccabue and B. E. Watts, Phys. Status Solidi, 1994, 141, K37.
10. E. Krogh Andersen, I. G. Krogh Andersen, J. Metcalf Johansen, K. E. Simonsen and E. Skou, Solid State Ionics, 1988, 28–30, 249.
11. K. E. Simonsen and E. Skou, in Solid State Protonic Conductors, ed. J. B. Goodenough, J. Jensen and M. Kleitz, Odense University Press, Odense, Denmark, 1983.
12. H. E. Rabinowitsch and W. C. Wood, Electrochemistry, 1933, 39, 562.
13. D. N. Stamires, J. Chem. Phys., 1962, 36, 3174.
14. I. R. Beattie and A. Dyer, J. Chem. Soc., Faraday Trans., 1957, 53, 61.
15. F. J. Jansen and R. A. Schoonheydt, J. Chem. Soc., Faraday Trans., 1973, 69, 1338.
16. E. Krogh Andersen, I. G. Krogh Andersen, E. Skou and S. Yde-Andersen, Solid State Ionics, 1986, 18/19, 1170.
17. N. Knudsen, E. Krogh Andersen, I. G. Krogh Andersen and E. Skou, Solid State Ionics, 1989, 35, 51.
18. D. C. Freeman and D. Stamires, J. Chem. Phys., 1961, 35, 799.
19. J. C. Giuntini, A. Jaboker and J. V. Zanchetta, Clay. Miner., 1985, 20, 347.
20. J. P. Ibar, Fundamentals of Thermally Stimulated Current, and Relaxation Map Analysis, ed. SLP Press, New York, 1993.
21. J. Vanderschueren and J. Gasiot, Thermally Stimulated Current, ed. P. Braunlich, Springer, Verlag, Berlin, 1979.
22. J. C. Giuntini, J. Vanderschueren, J. V. Zanchetta and F. Henn, Phys. Rev. B, 1994, 50, 12489.
23. G. Chabanis, V. Mouton, A. Abdoulaye, J. C. Giuntini and J. V. Zanchetta, Ionics, 1995, 1, 177.
24. A. K. Jonscher, Nature (London), 1977, 267, 673.
25. A. K. Jonscher, Dielectric Relaxation in Solids, Chesla Dielectric, London, 1983.
26. F. Buet, J. C. Giuntini, F. Henn and J. V. Zanchetta, Philos. Mag. B, 1992, 66, 77.
27. F. Salam, J. C. Giuntini, S. S. Soulayman and J. V. Zanchetta, Appl. Phys. A, 1996, 63.
28. D. H. Olson, Zeolites, 1995, 15, 439.
29. Y. I. Smolin, Y. F. Shepelev, I. K. Butikova and V. P. Pentranovskii, Kristallografiya., 1983, 28, 36.
30. G. N. D. Al-Ajdah, A. A. Al-Rished, B. Beagley, J. Dwyer, F. R. Fitch and T. K. Ibrahim, J. Inclusion Phenom., 1985, 3, 135.
31. G. Calestani, G. Bacca and G. D. Andreetti, Zeolites, 1987, 7, 54.
32. O. Glemser, Z. Anorg. Chem., 1944, 252, 305.
33. W. Marton, G. Ebert and F. H. Müller, Kolloid–Z.Z., Polym., 1971, 248, 986.
34. J. Kjaer and E. Skou, Solid State Ionics, 1990, 40/41, 121.
35. N. Cvjeticanin, S. Mentus and N. Petranovic, J. Chem. Soc., Faraday Trans., 1991, 79, 779.
36. R. Schoonheydt and J. B. Utterhoeven, Clay Miner., 1969, 8, 71.
37. F. J. Fripiat, A. Jelli, G. Poncellet and J. André, J. Phys. Chem., 1965, 69, 185.
38. R. Prost and J. Chaussidon, Clay Miner., 1969, 8, 143.
39. P. Pissis and D. Daoukaki-Diamanti, J. Chem. Solids, 1993, 54, 701.
40. R. Schoonheydt and W. De Wilde, J. Chem. Soc., Faraday Trans., 1974, 70, 2132.
41. U. Lohse, H. Stach, H. Hollnagel and W. Schirmer, Monatsber. Deutsche Akad. Wissenschaften Berlin, 1970, 12, 819.
42. K. T. No, H. Chon, T. Ree and M. S. John, J. Phys. Chem., 1981, 85, 2065.
43. E. Dempsey, J. Phys. Chem., 1969, 73, 3660.
44. L. Broussard and D. P. Shoemaker, J. Am. Chem. Soc., 1960, 82, 1041.
45. R. A. Schoonheydt, J. Phys., 1980, 6-41, 261.
46. J. C. Carru, P. Tabourier and J. M. Wacrenier, J. Chim. Phys., 1991, 88, 307.
47. G. Jones, J. Chem. Soc., Faraday Trans., 1985, 71, 2085.
48. S. W. S. McKerva and M. M. Hughes, J. Phys. D, 1975, 8, 1520.