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    On the Spontaneous Formation of Clathrate Hydrates at Water–Guest Interfaces
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    † TU Dortmund, Fakultät Physik/DELTA, Maria-Goeppert-Mayer-Str. 2, 44227 Dortmund, Germany
    ‡ European Synchrotron Radiation Facility, 6 rue Jules Horowitz, BP 220, 38043 Grenoble Cedex 9, France
    *E-mail: [email protected]
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2012, 116, 15, 8548–8553
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    https://doi.org/10.1021/jp211784w
    Published March 16, 2012
    Copyright © 2012 American Chemical Society
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    Abstract

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    The formation of hydrates, cage-like water-gas structures, is of tremendous importance both in industries and research. Although of major significance, the formation process is not completely understood so far. We present a comprehensive study of hydrate formation at liquid–liquid interfaces between water and isobutane, propane, carbon dioxide, and at the liquid–gas interface between water and xenon. We investigated the structure of these interfaces under quiescent conditions in situ by means of X-ray reflectivity measurements both inside and outside the zone of hydrate stability. At the interfaces between water and liquid alkanes, no evidence for a structural change was found. In contrast, the accumulation of guest molecules inside nanothick interfacial layers was observed at the water–xenon and liquid–liquid water–CO2 interfaces. We show that only those systems initially exhibiting such guest-enriched interfacial layers developed into macroscopic gas hydrates within our observation times (∼12 h). Therefore, these layers act as triggers for the spontaneous formation of macroscopic hydrates.

    Copyright © 2012 American Chemical Society

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    Figures showing the variation in reflectivity curves upon layer formation and the intensity breakdown after hydrate formation. This material is available free of charge via the Internet at http://pubs.acs.org.

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    This article is cited by 26 publications.

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    23. Niall J. English, Marco Lauricella, Simone Meloni. Massively parallel molecular dynamics simulation of formation of clathrate-hydrate precursors at planar water-methane interfaces: Insights into heterogeneous nucleation. The Journal of Chemical Physics 2014, 140 (20) https://doi.org/10.1063/1.4879777
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2012, 116, 15, 8548–8553
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jp211784w
    Published March 16, 2012
    Copyright © 2012 American Chemical Society
    Request reuse permissions

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