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Estimation of dissociation rate constant of CO 2 hydrate in water flow
Author(s) -
Fukumoto Ayako,
Sean WuYang,
Sato Toru,
Yamasaki Akihiro,
Kiyono Fumio
Publication year - 2015
Publication title -
greenhouse gases: science and technology
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.45
H-Index - 32
ISSN - 2152-3878
DOI - 10.1002/ghg.1469
Subject(s) - hydrate , dissociation (chemistry) , chemistry , gibbs free energy , thermodynamics , reaction rate constant , aqueous solution , solubility equilibrium , clathrate hydrate , solubility , activation energy , analytical chemistry (journal) , kinetics , chromatography , organic chemistry , physics , quantum mechanics
Dissociation processes of CO 2 hydrate under water flow conditions were investigated by experimental measurements and numerical calculation. Dissociation experiments were carried out with a CO 2 hydrate ball (diameter 10 mm) mounted in a flow cell, and the overall dissociation rate of CO 2 hydrate without bubble formation was measured under various conditions of temperature, pressure, and water flow rate. A linear phenomenological rate equation in the form of the product of the dissociation rate constant and the molar Gibbs free energy difference, between the hydrate phase and the ambient aqueous phase, was derived by considering the Gibbs free energy difference as the driving force for the dissociation. The molar Gibbs free energy difference was expressed by the logarithm of the ratio of the concentration of CO 2 dissolved in water at the hydrate surface to the solubility of CO 2 in the aqueous solution in equilibrium with the hydrate. The dissociation rate constant was determined from the experimental results of the overall dissociation rate combined with the numerical simulation results of the concentration profile of CO 2 constructed by the computational fluid dynamics (CFD) method. The obtained dissociation rate constant at the same pressure was found to be dependent on the temperature with the apparent activation energy of 97.51 k J/mol . A general form with product of the dissociation rate constant times driving force is proposed to calculate the dissociation rate of CO 2 hydrate in the water. © 2014 Society of Chemical Industry and John Wiley & Sons, Ltd

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