Journal
CHEMICAL ENGINEERING SCIENCE
Volume 81, Issue -, Pages 319-328Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ces.2012.07.006
Keywords
Semi-clathrate hydrate; TBAB; Thermodynamic model; Carbon dioxide; Methane; Nitrogen
Categories
Funding
- MINES ParisTech
- Agence Nationale de la Recherche (ANR) as part of the SECOHYA
- Orientation Strategique des Ecoles des Mines (OSEM)
- INSTITUT CARNOT MINES
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Prediction of phase equilibria of semi-clathrate hydrates has been very rarely investigated in the literature. In this work, a thermodynamic model is proposed for representation/prediction of phase equilibria of semi-clathrate hydrates of the CO2, CH4, or N-2+tetra-n-butylammonium bromide (TBAB) aqueous solution. For modeling the hydrate phase, the van der Waals-Platteeuw (vdW-P) solid solution theory is used, revised with two modifications for evaluations of Langmuir constants and vapor pressure of water in the empty hydrate lattice, in which these values are supposed to be a function of TBAB concentration in aqueous solution. The Peng-Robinson (PR-EoS) equation of state along with re-tuned parameters of Mathias-Copeman alpha function is applied for calculation of the fugacity of gaseous hydrate former. For determination of the activity coefficient of the non-electrolyte species in the aqueous phase, the Non-Random Two-Liquid (NRTL) activity model is used. To calculate the mean activity coefficients of the electrolyte portion, a correlation on the basis of existing osmotic coefficient and activity coefficient values is employed. It is shown that the presented model results are in acceptable agreement with the experimental semi-clathrate hydrate dissociation data investigated in this work. (C) 2012 Elsevier Ltd. All rights reserved.
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