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Molecular dynamics simulation of CO2 hydrates: Prediction of three phase coexistence line

Míguez Diaz, Jose Manuel and Conde, Maria Martin and Torré, Jean-Philippe and Blas, Felipe Jiménez and Piñeiro, Manuel M. and Vega, Carlos Molecular dynamics simulation of CO2 hydrates: Prediction of three phase coexistence line. (2015) Journal of Chemical Physics, 142 (12). 124505. ISSN 0021-9606

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Official URL: https://doi.org/10.1063/1.4916119


The three phase equilibrium line (hydrate-liquid water-liquid carbon dioxide) has been estimated for the water + carbon dioxide binary mixture using molecular dynamics simulation and the direct coexistence technique. Both molecules have been represented using rigid nonpolarizable models. TIP4P/2005 and TIP4P/Ice were used for the case of water, while carbon dioxide was considered as a three center linear molecule with the parameterizations of MSM, EPM2, TraPPE, and ZD. The influence of the initial guest occupancy fraction on the hydrate stability has been analyzed first in order to determine the optimal starting configuration for the simulations, paying attention to the influence of the two different cells existing in the sI hydrate structure. The three phase coexistence temperature was then determined for a pressure range from 2 to 500 MPa. The qualitative shape of the equilibrium curve estimated is correct, including the high pressure temperature maximum that determines the hydrate re-entrant behaviour. However, in order to obtain quantitative agreement with experimental results, a positive deviation from the classical Lorentz-Berthelot combining rules must be considered.

Item Type:Article
HAL Id:hal-01815919
Audience (journal):International peer-reviewed journal
Uncontrolled Keywords:
Institution:French research institutions > Centre National de la Recherche Scientifique - CNRS (FRANCE)
Other partners > Total (FRANCE)
Other partners > Universidad Complutense de Madrid - UCM (SPAIN)
Other partners > Université de Pau et des Pays de l'Adour - UPPA (FRANCE)
Other partners > Universidad de Huelva - UHU (SPAIN)
Other partners > Universidade de Vigo - UVIGO (SPAIN)
Laboratory name:
CESGA - MCIA (Mésocentre de Calcul Intensif Aquitain)
Deposited On:06 Feb 2019 11:29

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