Jump to main content
Jump to site search

Issue 19, 2019
Previous Article Next Article

Macroscopic defects upon decomposition of CO2 clathrate hydrate crystals

Author affiliations

Abstract

Micrometer- and submicrometer-sized pores and macroscopic defects like cracks and tubular channels can be found in a variety of clathrate hydrates (hydrates for short) during formation and decomposition. Their origin, their evolution in time, and their effect on hydrate decomposition kinetics are unclear. We used time-lapse micro computed tomography (μCT) in combination with temperature control and pressure monitoring to study the formation and evolution of pores and macroscopic defects in decomposing CO2 hydrates at subzero (Celsius) temperature. Our results suggest that the decomposition of hydrates is always accompanied by the formation of pores and an increase of the apparent hydrate volume by more than 3%. Hydrate decomposition often starts with the formation of cracks inside the hydrate and not necessarily at the free surface of the hydrate, which frequently remains intact for a long period and seems to be self-preserved in some regions. Decomposition spreads out from these cracks in a uniform fashion yielding a variety of macroscopic features. In some cases, the propagating decomposition front seems to get blocked by planar barriers inside the hydrate yielding regions with high resistance against decomposition. This, together with a generally heterogeneous distribution of decomposition resistant regions, challenges the shrinking core model of hydrate decomposition as well as the popular ice-rind theory used to explain the effect of self-preservation.

Graphical abstract: Macroscopic defects upon decomposition of CO2 clathrate hydrate crystals

Back to tab navigation

Supplementary files

Publication details

The article was received on 29 Dec 2018, accepted on 11 Apr 2019 and first published on 26 Apr 2019


Article type: Paper
DOI: 10.1039/C8CP07871H
Phys. Chem. Chem. Phys., 2019,21, 9694-9708
  • Open access: Creative Commons BY license
  •   Request permissions

    Macroscopic defects upon decomposition of CO2 clathrate hydrate crystals

    S. Arzbacher, N. Rahmatian, A. Ostermann, B. Massani, T. Loerting and J. Petrasch, Phys. Chem. Chem. Phys., 2019, 21, 9694
    DOI: 10.1039/C8CP07871H

    This article is licensed under a Creative Commons Attribution 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.

    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.

Search articles by author

Spotlight

Advertisements