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Theoretical study of phase transitions in Kr and Ar clathrate hydrates from structure II to structure I under pressure
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Subbotin, Oleg S., Adamova, Tatiana P., Belosludov, Rodion V., Mizuseki, Hiroshi, Kawazoe, Yoshiyuki, Kudoh, Jun-ichi, Rodger, P. Mark and Belosludov, Vladimir R. (2009) Theoretical study of phase transitions in Kr and Ar clathrate hydrates from structure II to structure I under pressure. Journal of Chemical Physics, Vol.131 (No.11). Article: 114507. doi:10.1063/1.3212965
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Official URL: http://dx.doi.org/10.1063/1.3212965
Abstract
The theory developed in our earlier papers is extended to predict dynamical and thermodynamic properties of clathrate structures by accounting for the possibility of multiple filling of cavities by guest molecules. The method is applied to the thermodynamic properties of argon and krypton hydrates, considering both structures I (sI) and II (sII), in which the small cages can be singly occupied and large cages of sII can be singly or doubly occupied. It was confirmed that the structure of the clathrate hydrate is determined by two main factors: intermolecular interaction between guest and host molecules and the configurational entropy. It is shown that for guests weakly interacting with water molecules, such as argon or krypton, the free energy of host lattices without the contribution of entropy is the main structure-determining factor for clathrate hydrates, and it is a cause of hydrate sII formation at low pressure with these guests. Explicit account of the entropy contribution in the Gibbs free energy allows one to determine the stability of hydrate phases and to estimate the line of structural transition from sII to sI in P-T plane. The structural transition between sII and sI in argon and krypton hydrates at high pressure is shown to be the consequence of increasing intermolecular interaction and the degree of occupancy of the large cavities. (C) 2009 American Institute of Physics. [doi: 10.1063/1.3212965]
| Item Type: | Journal Article | ||||
|---|---|---|---|---|---|
| Subjects: | Q Science > QC Physics | ||||
| Divisions: | Faculty of Science > Chemistry Faculty of Science > Centre for Scientific Computing |
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| Journal or Publication Title: | Journal of Chemical Physics | ||||
| Publisher: | American Institute of Physics | ||||
| ISSN: | 0021-9606 | ||||
| Official Date: | 21 September 2009 | ||||
| Dates: |
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| Volume: | Vol.131 | ||||
| Number: | No.11 | ||||
| Number of Pages: | 8 | ||||
| Page Range: | Article: 114507 | ||||
| DOI: | 10.1063/1.3212965 | ||||
| Status: | Peer Reviewed | ||||
| Publication Status: | Published | ||||
| Access rights to Published version: | Restricted or Subscription Access | ||||
| Funder: | Russian Foundation for Basic Research, INTAS | ||||
| Grant number: | 08-03-00191, 03-51-5537 |
Data sourced from Thomson Reuters' Web of Knowledge
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