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Low-temperature thermodynamic study of the metastable empty clathrate hydrates using molecular simulations

Par Conseil national de recherches du Canada

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DOITrouver le DOI : https://doi.org/10.1021/acsearthspacechem.9b00009
AuteurRechercher : Identifiant ORCID : https://orcid.org/0000-0002-1300-2801; Rechercher : 1; Rechercher : Identifiant ORCID : https://orcid.org/0000-0001-6752-5766
Affiliation
  1. Conseil national de recherches du Canada. Aérospatiale
FormatTexte, Article
Sujetempty clathrate hydrates; thermodynamics; structure; p−V−T data; molecular dynamics; isobaric expansivity; isobaric heat capacity
Résumé
The thermodynamics of metastable empty sI-clathrate hydrates are probed over broad temperature and pressure ranges, 100 ≤ T (K) ≤ 220 and 1 ≤ p (bar) ≤ 5000, respectively, by large-scale simulations and compared with experimental data at 1 bar. The whole p–V–T surface obtained is fitted by the universal form of the Parsafar and Mason equation of state with an accuracy of 99.7–99.9%. Framework deformation brought about by the applied temperature follows a parabolic law, and there is a critical temperature above which the isobaric thermal expansion becomes negative, ranging from 194.7 K at 1 bar to 166.2 K at 5000 bar. That response to the applied (p, T) field is analyzed in terms of angle and distance descriptors of a classical tetrahedral structure and observed to occur essentially by means of angular alteration for (p, T) > (2000 bar, 200 K). The length of the hydrogen bonds responsible for framework integrity is insensitive to the thermodynamic conditions and its average value is ̅r(O-H)=0.25 nm.
Date de publication
Maison d’éditionAmerican Chemical Society
Dans
  • ACS Earth and Space Chemistry 3, nº 5 : 789–799.
Langueanglais
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Identificateur de l’enregistrementf30edd8f-3d02-4f90-a845-2d00542d95fd
Enregistrement créé2021-03-19
Enregistrement modifié2021-03-19
Date de modification :