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The rheology of collapsing zeolites amorphized by temperature and pressure

Nature Materials volume 2, pages 622–629 (2003)Cite this article

Abstract

Low-density zeolites collapse to the rigid amorphous state at temperatures that are well below the melting points of crystals of the same composition but of conventional density. Here we show, by using a range of experimental techniques, how the phenomenon of amorphization is time dependent, and how the dynamics of order–disorder transitions in zeolites under temperature and pressure are equivalent. As a result, thermobaric regions of instability can be charted, which are indicative of polyamorphism. Moreover, the boundaries of these zones depend on the rate at which temperature or pressure is ramped. By directly comparing the rheology of collapse with structural relaxation in equivalent melts, we conclude that zeolites amorphize like very strong liquids and, if compression occurs slowly, this is likely to lead to the synthesis of perfect glasses.

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Figure 1: Scanning electron micrographs following the changing morphology of zeolite collapse; 300-nm bars relate the different magnifications.
Figure 2: Measuring the time dependence of temperature-induced zeolite collapse by using XRD, DSC and SAXS.
Figure 3: Measuring the time dependence of pressure-induced zeolite collapse by using XRD.
Figure 4: Temperature–pressure relations for the amorphization of zeolite A and zeolite Y.
Figure 5: Rheological characteristics of zeolite amorphization induced by temperature and pressure.

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Acknowledgements

We thank C. A. Angell, M. H. Cohen, D. B. Dingwell, S. Webb, K. Walters and M. Wilding for discussions. The experimental work was financially supported from the UK Engineering and Physical Sciences Research Council and X-ray facilities at the Synchrotron Radiation Source, Daresbury Laboratory, UK. F.M. thanks the EU Framework 5 Programme for a studentship.

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Authors and Affiliations

  1. Institute of Mathematical and Physical Sciences, University of Wales, Aberystwyth, SY23 3BZ, UK

    G. N. Greaves & F. Meneau

  2. Royal Institution of Great Britain, 21 Albemarle Street, London, W1X 4BS, UK

    F. Meneau & G. Sankar

  3. Department of Chemistry, De Montfort University, Leicester, LE1 9BH, UK

    A. Sapelkin

  4. Department of Chemistry, University of Keele, Staffordshire, ST5 5BG, UK

    L. M. Colyer

  5. Institute of Biological Studies, University of Wales, Aberystwyth, SY23 3DA, UK

    I. ap Gwynn & S. Wade

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Correspondence to G. N. Greaves.

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Greaves, G., Meneau, F., Sapelkin, A. et al. The rheology of collapsing zeolites amorphized by temperature and pressure. Nature Mater 2, 622–629 (2003). https://doi.org/10.1038/nmat963

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