Skip to main content
SpringerLink
Log in

An investigation into the crystallization of low-silica X zeolite

  • Published:
Journal of Porous Materials Aims and scope Submit manuscript

Abstract

The crystallization of low-silica X (LSX) zeolite with FAU topology was examined under hydrothermal synthesis conditions. PXRD was employed to follow the evolution of the long-range ordering of the gel. Raman spectra provided information on various ring and cage species existing in the gel. 27Al and 29Si solid-state NMR spectroscopy was utilized to monitor the change in local environment of tetrahedral sites. The results indicate that an amorphous aluminosilicate phase was formed immediately upon mixing different reactive species. Hydrothermal treatment led to the formation of sodalite-cage like species and the species with larger cavities, joint four-member rings (4Rs) and branched 4Rs, which are the structural building units of the FAU framework. These units were assembled into the crystalline structure of LSX zeolite. 23Na and 39K solid-state NMR results show that the transformation process was accompanied by the changes of the local structure of hydrated Na+ and K+ ions. The two types of cations may work synergistically to template the crystallization of LSX zeolite.

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

Scheme 1
Fig. 1
Fig. 2
Scheme 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  1. R.J. Davis, J. Catal. 216, 396 (2003)

    Article  CAS  Google Scholar 

  2. R.A. Schoonheydt, P. Geerlings, E.A. Pidko, R.A. van Santen, J. Mater. Chem. 22, 18705 (2012)

    Article  CAS  Google Scholar 

  3. B. Smit, T.L.M. Maesen, Chem. Rev. 108, 4125 (2008)

    Article  CAS  Google Scholar 

  4. Ch. Baerlocher, L.B. McCusker, Database of zeolite structures. http://www.iza-structure.org/databases/

  5. L. Zhang, A.N.C. Laak, P.E. Jongh, K.P. Jong, Microporous Mesoporous Mater. 126, 115 (2009)

    Article  CAS  Google Scholar 

  6. Y. Lee, S.W. Carr, J.B. Parise, Chem. Mater. 10, 2561 (1998)

    Article  CAS  Google Scholar 

  7. T. Frising, P. Leflaive, Microporous Mesoporous Mater. 114, 27 (2008)

    Article  CAS  Google Scholar 

  8. P. Kovacheva, K. Arishtirova, A. Predoeva, React. Kinet. Catal. Lett. 79, 149 (2003)

    Article  CAS  Google Scholar 

  9. A.F. Ojo, F.R. Fitch, M. Bülow, C.S. Gittleman, S.R. Jale, US Patent 6596256 (2003)

  10. R.T. Yang, N.D. Hutson, US Patent 6780806 (2004)

  11. R. Jasra, N. Choudary, S. Bhat, Ind. Eng. Chem. Res. 35, 4221 (1996)

    Article  CAS  Google Scholar 

  12. E. Basaldella, J. Tara, Zeolites 15, 243 (1995)

    Article  CAS  Google Scholar 

  13. G. Vitale, L.M. Bull, R.E. Morris, A.K. Cheetham, B.H. Toby, C.G. Coe, J.E. MacDougall, J. Phys. Chem. 99, 16087 (1995)

    Article  CAS  Google Scholar 

  14. D. Schaefer, D. Favre, M. Wilhelm, S. Weigel, B.J. Chmelka, Am. Chem. Soc. 119, 9252 (1997)

    Article  CAS  Google Scholar 

  15. J. Plevert, F. Di Renzo, F. Fajula, G. Chiari, J. Phys. Chem. B 101, 10340 (1997)

    Article  CAS  Google Scholar 

  16. M. Feuerstein, G. Engelhardt, P. McDaniel, J. MacDougall, T. Gaffney, Microporous Mesoporous Mater. 26, 27 (1998)

    Article  CAS  Google Scholar 

  17. S.R. Jale, M. Büow, F.R. Fitch, N. Perelman, D. Shen, J. Phys. Chem. B 104, 5272 (2000)

    Article  CAS  Google Scholar 

  18. US Patent, 6, 264, 881

  19. S. Caldarelli, A. Buchholz, M. Hunger, J. Am. Chem. Soc. 123, 7118 (2001)

    Article  CAS  Google Scholar 

  20. J. Plévert, T. Okubo, Y. Wada, M. O’Keeffe, T. Tatsumi, Chem. Commun. 20, 2112 (2001)

    Article  Google Scholar 

  21. V.B. Kazansky, M. Bülow, E. Tichomirova, Adsorption 7, 291 (2001)

    Article  CAS  Google Scholar 

  22. D. Shen, M. Bülow, S.R. Jale, F.R. Fitch, A.F. Ojo, Microporous Mesoporous Mater. 48, 211 (2001)

    Article  CAS  Google Scholar 

  23. T. Loeser, D. Freude, G.T.P. Mabande, W. Schwieger, Chem. Phys. Lett. 370, 32 (2003)

    Article  CAS  Google Scholar 

  24. J.C. Buhl, M. Gerstmann, W. Lutz, A.Z. Ritzmann, Anorg. Allg. Chem. 630, 604 (2004)

    Article  CAS  Google Scholar 

  25. M. Romero, J. Gomez, G. Ovejero, A. Rodriguez, Mater. Res. Bull. 39, 389 (2004)

    Article  CAS  Google Scholar 

  26. J.E. Readman, C.P. Grey, M. Ziliox, L.M. Bull, A. Samoson, Solid State Nucl. Magn. Reson. 26, 153 (2004)

    Article  CAS  Google Scholar 

  27. V.B. Kazansky, N.A. Sokolova, M. Bülow, Microporous Mesoporous Mater. 67, 283 (2004)

    Article  CAS  Google Scholar 

  28. N. Sokolova, V. Kazanskii, Kinet. Catal. 46, 879 (2005)

    Article  CAS  Google Scholar 

  29. P. Khemthong, J. Wittayakun, S. Prayoonpokarach, Suranaree J. Sci. Technol. 14, 367 (2007)

    Google Scholar 

  30. A. Wozniak, B. Marler, K. Angermund, H. Gies, Chem. Mater. 20, 5968 (2008)

    Article  CAS  Google Scholar 

  31. D. Schneider, H. Toufar, A. Samoson, D. Freude, Solid State Nucl. Magn. Reson. 35, 87 (2009)

    Article  CAS  Google Scholar 

  32. H. Guesmi, P. Massiani, H. Nouali, J.L. Paillaud, Microporous Mesoporous Mater. 159, 87 (2012)

    Article  CAS  Google Scholar 

  33. G.H. Kuhl, Zeolites 7, 451 (1987)

    Article  CAS  Google Scholar 

  34. M. Iwama, Y. Suzuki, J. Plévert, K. Itabashi, M. Ogura, T. Okubo, Cryst. Growth Des. 10, 3471 (2010)

    Article  CAS  Google Scholar 

  35. G. Xiong, Y. Yu, Z. Feng, Q. Xin, F.S. Xiao, C. Li, Microporous Mesoporous Mater. 42, 317 (2001)

    Article  CAS  Google Scholar 

  36. F. Fan, Z. Feng, G. Li, K. Sun, P. Ying, C. Li, Chem. Eur. J. 14, 5125 (2008)

    Article  CAS  Google Scholar 

  37. F. Fan, Z. Feng, C. Li, Chem. Soc. Rev. 39, 4794 (2010)

    Article  CAS  Google Scholar 

  38. A. Depla, E. Verheyen, A. Veyfeyken, E. Gobechiya, T. Hartmann, R. Schaefer, J.A. Martens, C.E.A. Kirschhock, Phys. Chem. Chem. Phys. 13, 13730 (2011)

    Article  CAS  Google Scholar 

  39. B. Lok, T. Cannan, C. Messina, Zeolites 3, 282 (1983)

    Article  CAS  Google Scholar 

  40. S. Le Caér, F. Brunet, C. Chatelain, D. Durand, V. Dauvois, T. Charpentier, JPh Renault, J. Phys. Chem. C 116, 4748 (2012)

    Article  Google Scholar 

  41. K. Eichele, R.E. Wasylishen, v. 1.19.15 edn. (2009)

  42. A. Inayat, I. Knoke, E. Spiecker, W. Schwieger, Angew. Chem. Int. Ed. 51, 1962 (2012)

    Article  CAS  Google Scholar 

  43. P.K. Dutta, K.M. Rao, J.Y. Park, J. Phys. Chem. 95, 6654 (1991)

    Article  CAS  Google Scholar 

  44. P.K. Dutta, D. Shieh, M. Puri, Zeolites 8, 306 (1988)

    Article  CAS  Google Scholar 

  45. C. Bremard, M. Le Maire, J. Phys. Chem. 97, 9695 (1993)

    Article  CAS  Google Scholar 

  46. A. Miecznikowski, J. Hanuza, Zeolites 5, 188 (1985)

    Article  CAS  Google Scholar 

  47. J. Twu, P.K. Dutta, C.T. Kresge, Zeolites 11, 672 (1991)

    Article  CAS  Google Scholar 

  48. P.K. Dutta, D. Shieh, M.J. Puri, Phys. Chem. 91, 2332 (1987)

    Article  CAS  Google Scholar 

  49. P.K. Dutta, J. Twu, J. Phys. Chem. 95, 2498 (1991)

    Article  CAS  Google Scholar 

  50. W. Yan, X. Song, R. Xu, Microporous Mesoporous Mater. 123, 50 (2009)

    Article  CAS  Google Scholar 

  51. T. Cheng, J. Xu, X. Li, Y. Li, B. Zhang, W. Yan, J. Yu, H. Sun, F. Deng, R. Xu, Microporous Mesoporous Mater. 152, 190 (2012)

    Article  CAS  Google Scholar 

  52. P. Bodart, J.B. Nagy, Z. Gabelica, E.G. Derouane, J. Chim. Phys. 83, 777 (1986)

    CAS  Google Scholar 

  53. L. Ren, C. Li, F. Fan, Q. Guo, D. Liang, Z. Feng, C. Li, S. Li, F.S. Xiao, Chem. Eur. J. 17, 6162 (2011)

    Article  CAS  Google Scholar 

  54. C. Doremieux-Morin, C. Martin, J.M. Bregeault, J. Fraissard, Appl. Catal. 77, 149 (1991)

    Article  CAS  Google Scholar 

  55. G.E. Maciel, C.E. Bronnimann, R.C. Zeigler, I.S. Chuang, D.R. Kinney, E.A. Keiter, Adv. Chem. Ser. 234, 269 (1994)

    Article  CAS  Google Scholar 

  56. C.C. Liu, G.E. Maciel, J. Am. Chem. Soc. 118, 5103 (1996)

    Article  CAS  Google Scholar 

  57. M. Ogura, Y. Kawazu, H. Takahashi, T. Okubo, Chem. Mater. 15, 2661 (2003)

    Article  CAS  Google Scholar 

  58. E. Lippmaa, M. Maegi, A. Samoson, M. Tarmak, G. Engelhardt, J. Am. Chem. Soc. 103, 4992 (1981)

    Article  CAS  Google Scholar 

  59. H. Koller, G. Engelhardt, A.P.M. Kentgens, J. Sauer, J. Phys. Chem. 98, 1544 (1994)

    Article  CAS  Google Scholar 

  60. I. Hannus, I. Kiricsi, P. Lentz, J. Nagy, Colloids Surf. A 158, 29 (1999)

    Article  CAS  Google Scholar 

  61. A. Seidel, U. Tracht, B. Boddenberg, J. Phys. Chem. 100, 15917 (1996)

    Article  CAS  Google Scholar 

  62. I.L. Moudrakovski, J.A. Ripmeester, J. Phys. Chem. B 111, 491 (2007)

    Article  CAS  Google Scholar 

  63. A.T. Durant, K.J. MacKenzie, H. Maekawa, Dalton Trans. 40, 4865 (2011)

    Article  CAS  Google Scholar 

  64. V.F. Barbosa, K.J. MacKenzie, Mater. Lett. 57, 1477 (2003)

    Article  CAS  Google Scholar 

  65. M. Smith, Clays Clay Miner. 40, 253 (1992)

    Article  Google Scholar 

Download references

Acknowledgments

Y. H. thanks the Natural Science and Engineering Research Council of Canada for a Discovery grant. Access to the 900 MHz NMR spectrometer was provided by the Canadian National Ultrahigh Field NMR Facility for Solids (http://nmr900.ca). We thank Dr. V. Terskikh for acquiring 39K NMR spectra and Mr. P. He for 39K spectral simulation. We also thank Prof. Yang Song for the access of a Raman spectrometer. This work was funded by the Natural Science and Engineering Research Council of Canada (2012).

Conflict of interest

The authors declare that they have no conflict of interest.

Author information

Authors and Affiliations

  1. Department of Chemistry, The University of Western Ontario, London, ON, N6A 5B7, Canada

    Lu Zhang & Yining Huang

Authors
  1. Lu Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Yining Huang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Yining Huang.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, L., Huang, Y. An investigation into the crystallization of low-silica X zeolite. J Porous Mater 22, 843–850 (2015). https://doi.org/10.1007/s10934-015-9957-1

Download citation

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10934-015-9957-1

Keywords

Search

Navigation