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Nonequilibrium Thermodynamics of Hydrate Growth on a Gas-Liquid Interface

Fu, Xiaojing and Cueto-Felgueroso, Luis and Juanes, Ruben (2018) Nonequilibrium Thermodynamics of Hydrate Growth on a Gas-Liquid Interface. Physical Review Letters, 120 (14). Art. No. 144501. ISSN 0031-9007. doi:10.1103/physrevlett.120.144501.

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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.

Item Type:Article
Related URLs:
URLURL TypeDescription
Fu, Xiaojing0000-0001-7120-704X
Juanes, Ruben0000-0002-7370-2332
Additional Information:© 2018 American Physical Society. Received 28 September 2017; revised manuscript received 16 January 2018; published 2 April 2018. We thank Carolyn Ruppel and William Waite from USGS for insightful discussions. This work was funded in part by the U.S. Department of Energy (Awards No. DE-FE0013999 and No. DE-SC0018357). L. C. F. acknowledges funding from the Spanish Ministry of Economy and Competitiveness (Grants No. RYC-2012-11704 and No. CTM2014-54312-P). L. C. F. and R. J. acknowledge funding from the MIT International Science and Technology Initiatives, through a Seed Fund grant.
Funding AgencyGrant Number
Department of Energy (DOE)DE-FE0013999
Department of Energy (DOE)DE-SC0018357
Ministerio de Economía, Industria y Competitividad (MINECO)RYC-2012-11704
Ministerio de Economía, Industria y Competitividad (MINECO)CTM2014-54312-P
Massachusetts Institute of Technology (MIT)UNSPECIFIED
Issue or Number:14
Record Number:CaltechAUTHORS:20200902-151231348
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:105230
Deposited By: Tony Diaz
Deposited On:08 Sep 2020 23:25
Last Modified:16 Nov 2021 18:41

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