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Journal of Materials Science

, Volume 26, Issue 6, pp 1443–1453 | Cite as

The formation of β′-sialon from a montmorillonite-polyacrylonitrile composite by carbothermal reduction: an NMR, TGA, XRD and EM study

  • T. Bastow
  • S. G. Hardin
  • T. W. Turney
Papers

Abstract

The products of carbothermal reduction in N2 of a nanocomposite between dodecylammonium-exchanged montmorillonite and polyacrylonitrile (PAN) have been studied by solid-state 27Al and 29SiNMR spectroscopy, X-ray diffraction, transmission electron microscopy and thermogravimetry. Comparison with analogous reactions involving sodium-exchanged montmorillonite and dodecylammonium-exchanged montmorillonite (without PAN) shows that in the presence of PAN, the formation of silica, cordierite or mullite is almost completely suppressed. The only crystalline phase detected between 1000 and 1300 °C was a β′-sialon, having a much higher Si∶Al ratio (7.05∶1) than that of the precursor clay (2.44∶1). Reduction of the octahedral AlO6 begins near 1200 °C, forming increasing amounts of Al(N,O)4 tetrahedra with temperature, so that by 1600 °C, complete reduction to AlN4 (i.e. bulk AlN) has occurred. In contrast, reduction of the tetrahedral SiO4 is appreciable at 1100 °C, and is almost complete (SiN4 tetrahedra only) by 1200 °C. No intermediate Si(N,0)4 environments are found. By 1600 °C, only the SiC4 environment (i.e. bulk SiC) remains. A mechanism is suggested, involving the formation of alternating slabs of an amorphous aluminosilicate and carbon at 1000 °C, followed by diffusion of silicon from the outer regions of the aluminosilicate band towards the centre, and sequential reduction of Si(OSi)4 and Si(OSi)3 (OAl) groups.

Keywords

Transmission Electron Microscopy Montmorillonite Aluminosilicate Cordierite Outer Region 
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.

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References

  1. 1.
    K. H. Jack, in ldNon-Oxide Technical and Engineering Ceramics”, edited by Stuart Hampshire (Elsevier, 1986) p. 1.Google Scholar
  2. 2.
    I. J. McColm,in “Ceramic Science for Materials Technologists” (Leonard Hill, New York, 1983).Google Scholar
  3. 3.
    K. H. Jack, in “High Technology Ceramics”, Vol. 3 of “Ceramics & Civilization”, edited by W. D. Kingery (American Chemical Society, 1986).Google Scholar
  4. 4.
    Idem, J. Mater. Sci. 11 (1976) 1135.CrossRefGoogle Scholar
  5. 5.
    A. J. Moulson, ibid. 14 (1979) 1017.CrossRefGoogle Scholar
  6. 6.
    J. B. Baldo, V. C. Pandolfelli and J. R. Casarini, in “Ceramic Powders”, edited by P. Vincenzini (Elsevier, Amsterdam, 1983) pp. 437–444.Google Scholar
  7. 7.
    I. L. Boyarina, A. B. Puchkov, A. M. Gaurish, Z. D. Zhukova and E. V. Degtyareva, Refractories (Engl. Transl.) 23 (1982) 191.Google Scholar
  8. 8.
    C. J. Spacie, in “Non-oxide Technical and Engineering Ceramics”, edited by Stuart Hampshire (Elsevier Applied Science, 1983) pp. 133–147.Google Scholar
  9. 9.
    J. Mukerji and S. Bandyopadhyay, Adv. Ceram. Mater. 3 (1988) 369.CrossRefGoogle Scholar
  10. 10.
    J.-G. Lee and I. B. Cutler, Amer. Ceram. Soc. Bull. 58 (1979) 869.Google Scholar
  11. 11.
    S. Bandyopadhyay and J. Mukerji, Adv. Ceram. Mater. 3 (1988) 328.CrossRefGoogle Scholar
  12. 12.
    S. A. Siddiqi, I. Higgins and A. Hendry, in “Non-oxide Technical and Engineering Ceramics”, edited by Stuart Hampshire (Elsevier Applied Science, 1983) pp. 119–132.Google Scholar
  13. 13.
    F. K. Van Dijen, R. Metsalaar and C. A. M. Siskens, J. Amer. Ceram. Soc. 68 (1985) 16.CrossRefGoogle Scholar
  14. 14.
    I. Higgins and A. Hendry, Proc. Br. Ceram. Soc. 38 (1986) 163.Google Scholar
  15. 15.
    M. E. Bowden, K. J. D. Mackenzie and J. H. Johnston, in “Ceramic Developments”, edited by C. C. Sorrell and B. Ben-Nissan (Trans Tech Publications, 1988).Google Scholar
  16. 16.
    Y. Sugahara, K. Kuroda and C. Kato, Ceram. Int. 14 (1988) 1.CrossRefGoogle Scholar
  17. 17.
    Idem, J. Mater. Sci. 23 (1988) 3572.CrossRefGoogle Scholar
  18. 18.
    Y. Sugahara, K. Sugimoto, K. Kuroda and C. Kato, Yogyo Kyokaishi 94 (1986) 48.CrossRefGoogle Scholar
  19. 19.
    R. H. Meinhold, K. J. D. Mackenzie and I. W. M. Brown, J. Mater. Sci. Lett. 4 (1985) 163.CrossRefGoogle Scholar
  20. 20.
    E. Lippmaa, A. Samoson and M. Magi, J. Amer. Chem. Soc. 108 (1986) 1730.CrossRefGoogle Scholar
  21. 21.
    D. Tilak, B. Tenakoon, J. M. Thomas, W. Jones, T. A. Carpenter and S. Ramdas, J. Chem. Soc. Faraday Trans. 1 82 (1986) 545.CrossRefGoogle Scholar
  22. 22.
    J. G. Thompson, Clay Miner. 19 (1984) 229.CrossRefGoogle Scholar
  23. 23.
    D. Tilak, B. Tenakoon, W. Jones and J. M. Thomas, J. Chem. Soc. Faraday Trans. 1 82 (1986) 3081.CrossRefGoogle Scholar
  24. 24.
    E. Lippmaa, M. Magi, A. Samoson, G. Engelhardt and A. R. Grimmer, J. Amer. Chem. Soc. 102 (1980) 4889.CrossRefGoogle Scholar
  25. 25.
    M. Magi, E. Lippmaa, A. Samoson, G. Engelhardt and A. R. Grimmer, J. Phys. Chem. 88 (1984) 1518.CrossRefGoogle Scholar
  26. 26.
    J. B. Murdoch, J. F. Stebbins and I. S. E. Carmichael, Amer. Mineral. 70 (1985) 332.Google Scholar
  27. 27.
    C. A. Weiss Jr, S. P. Altaner and R. J. Kirkpatrick, ibid. 72 (1987) 935.Google Scholar
  28. 28.
    J. Sanz and J. M. Serratosa, J. Amer. Chem. Soc. 106 (1984) 4790.CrossRefGoogle Scholar
  29. 29.
    I. W. M. Brown, K. J. D. Mackenzie and R. H. Meinhold, J. Mater. Sci. 22 (1987) 3265.CrossRefGoogle Scholar
  30. 30.
    J. Sanz, A. Madani, J. M. Serratosa, J. S. Moya and S. Aza, J. Amer. Ceram. Soc. 71 (1988) C418.CrossRefGoogle Scholar
  31. 31.
    C. A. Fyfe, J. M. Thomas, J. Klinowski and G. C. Gobbi, Angew. Chem. Int. Ed. Engl. 22 (1983) 259.CrossRefGoogle Scholar
  32. 32.
    J. Klinowski, J. M. Thomas, D. P. Thompson, P. Korgul, K. H. Jack, C. A. Fyfe and G. C. Gobbi, Polyhedron 3 (1984) 1267.CrossRefGoogle Scholar
  33. 33.
    R. S. Aujla, G. Leng-ward, M. H. Lewis, E. F. W. Seymour, G. A. Styles and G. W. West, Phil. Mag. B 54 (1986) L51.CrossRefGoogle Scholar
  34. 34.
    T. Taki, M. Inui, K. Okamura and M. Sato, J. Mater. Sci. Lett. 8 (1989) 918.CrossRefGoogle Scholar
  35. 35.
    M. I. Attala, L. A. Bruce, S. I. Hodgson, T. W. Turney, M. A. Wilson and B. D. Batts, Fuel 69 (1990) 725.CrossRefGoogle Scholar
  36. 36.
    C. Doblin, personal communication (1989).Google Scholar
  37. 37.
    S. A. Siddiqi and A. Hendry, J. Mater. Sci. 20 (1985) 3230.CrossRefGoogle Scholar
  38. 38.
    J. W. Earley, I. H. Milne and W. J. McVeagh, Amer. Mineral. 38 (1953) 770.Google Scholar
  39. 39.
    “Chemistry of Clays and Clay Minerals”, edited by A. C. D. Newman, Mineralogical Society Monograph No. 6 (Longman, 1987) pp. 321, 355.Google Scholar
  40. 40.
    Ibid., p. 312.Google Scholar
  41. 41.
    Y. Sugahara, K. Kuroda and C. Kato, J. Amer. Ceram. Soc. 67 (1984) C247.CrossRefGoogle Scholar
  42. 42.
    J. W. Earley, B. B. Osthaus and I. H. Milne, Amer. Mineral. 38 (1953) 707.Google Scholar
  43. 43.
    W. F. Bradley and R. E. Grim, ibid. 36 (1951) 182.Google Scholar
  44. 44.
    R. E. Grim and G. Kulbicki, ibid. 46 (1961) 1329.Google Scholar
  45. 45.
    G. Kulbicki, Clays Clay Miner. 5 (1958) 144.CrossRefGoogle Scholar
  46. 46.
    G. Engelhardt, D. Zeigan, H. Jancke, D. Hoebbel and W. Wieker, Z. Anorg. Allg. Chem. 418 (1975) 17.CrossRefGoogle Scholar
  47. 47.
    G. Engelhardt, H. Jancke, D. Hoebbel and W. Wieker, Z. Chem. 14 (1974) 109.CrossRefGoogle Scholar
  48. 48.
    I. W. M. Brown, K. J. D. Mackenzie, M. E. Bowden and R. H. Meinhold, J. Amer. Ceram. Soc. 68 (1985) 298.CrossRefGoogle Scholar
  49. 49.
    J. V. Smith and C. S. Blackwell, Nature 303 (1983) 223.CrossRefGoogle Scholar
  50. 50.
    G. R. Finlay, J. S. Hartman, M. F. Richardson and B. L. Williams, J. Chem. Soc. Commun. (1985) 159.Google Scholar
  51. 51.
    M. A. Wilson, in “NMR Techniques and Applications in Geochemistry and Soil Chemistry” (Pergamon, 1987) p. 117.Google Scholar
  52. 52.
    N. D. Butler, R. Dupree and M. H. Lewis, J. Mater. Sci. Lett. 3 (1984) 469.CrossRefGoogle Scholar
  53. 53.
    I. Higgins and A. Hendry, Trans. J. Br. Ceram. Soc. 85 (1986) 161.Google Scholar

Copyright information

© Chapman and Hall Ltd. 1991

Authors and Affiliations

  • T. Bastow
    • 1
  • S. G. Hardin
    • 1
  • T. W. Turney
    • 1
  1. 1.CSIRO Division of Materials Science and TechnologyClaytonAustralia

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