Jump to main content
Jump to site search

Issue 7, 2015
Previous Article Next Article

Temperature-induced amorphisation of hexagonal ice

Author affiliations

Abstract

We systematically studied the competition between polymorphic transformations and amorphisation of hexagonal ice on isobaric heating from 77 K to 155–170 K at pressures between 0.50 and 1.00 GPa. This competition is analysed here systematically by in situ dilatometry and ex situ X-ray diffraction and calorimetry. Volume vs. temperature curves were analysed using a novel fitting approach in order to understand the underlying mechanism. Hexagonal ice undergoes solid-state-transformation to ice IX/III at 0.50 and 0.60 GPa and to a mixture of ices IX/III and IV at 0.70 and 0.80 GPa. Possibly a tiny fraction of amorphous intermediate is transiently formed in this pressure range. At 0.85 GPa the amorphisation process becomes competitive, and leads to very high-density amorphous ice (VHDA) as by-product. At 0.90 and 0.95 GPa VHDA is the main product and at 1.00 GPa only VHDA is found. This represents the first observation of temperature-induced amorphisation (TIA) for hexagonal ice using diffraction methods. Our analysis suggests TIA to be a first-order phase transition which, by contrast to pressure-induced amorphisation (PIA), does not involve a precursor process. We suggest interpreting TIA as thermodynamic melting of ice followed by immediate vitrification rather than as mechanical collapse of hexagonal ice. The activation energies for amorphisation and polymorphic transformation are equal at ∼0.75 GPa. At 1.00 GPa the activation energy for amorphisation of hexagonal ice is lower by about 6 kJ mol−1 than the activation energy for polymorphic transitions.

Graphical abstract: Temperature-induced amorphisation of hexagonal ice

Back to tab navigation

Article information


Submitted
01 Dec 2014
Accepted
13 Jan 2015
First published
13 Jan 2015

This article is Open Access

Phys. Chem. Chem. Phys., 2015,17, 5403-5412
Article type
Paper
Author version available

Temperature-induced amorphisation of hexagonal ice

P. H. Handle and T. Loerting, Phys. Chem. Chem. Phys., 2015, 17, 5403
DOI: 10.1039/C4CP05587J

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material and it is not used for commercial purposes.

Reproduced material should be attributed as follows:

  • For reproduction of material from NJC:
    [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
  • For reproduction of material from PCCP:
    [Original citation] - Published by the PCCP Owner Societies.
  • For reproduction of material from PPS:
    [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
  • For reproduction of material from all other RSC journals:
    [Original citation] - Published by The Royal Society of Chemistry.

Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.


Social activity

Search articles by author

Spotlight

Advertisements