Nonequilibrium Thermodynamics of Hydrate Growth on a Gas-Liquid Interface
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PhysRevLett.120.144501.pdf
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Author(s) • •
Fu, Xiaojing
Cueto-Felgueroso Landeira, Luis
Juanes, Ruben
Date Issued
April 2018
Journal
Physical Review Letters
Publisher
American Physical Society
Citation
Fu, Xiaojing et al. "Nonequilibrium Thermodynamics of Hydrate Growth on a Gas-Liquid Interface." Physical Review Letters 120, 14 (April 2018): 144501 © 2018 American Physical Society
Version
Final published version
Abstract
We develop a continuum-scale phase-field model to study gas-liquid-hydrate systems far from thermodynamic equilibrium. We design a Gibbs free energy functional for methane-water mixtures that recovers the isobaric temperature-composition phase diagram under thermodynamic equilibrium conditions. The proposed free energy is incorporated into a phase-field model to study the dynamics of hydrate formation on a gas-liquid interface. We elucidate the role of initial aqueous concentration in determining the direction of hydrate growth at the interface, in agreement with experimental observations. Our model also reveals two stages of hydrate growth at an interface—controlled by a crossover in how methane is supplied from the gas and liquid phases—which could explain the persistence of gas conduits in hydrate-bearing sediments and other nonequilibrium phenomena commonly observed in natural methane hydrate systems.
MIT Department
Massachusetts Institute of Technology. Department of Civil and Environmental Engineering
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DOI of Published Version
https://doi.org/10.1103/PhysRevLett.120.144501