Nonequilibrium Thermodynamics of Hydrate Growth on a Gas-Liquid Interface

Fu, Xiaojing; Cueto-Felgueroso, Luis; Juanes, Ruben

doi:10.1103/physrevlett.120.144501

Title: Nonequilibrium Thermodynamics of Hydrate Growth on a Gas-Liquid Interface

Journal Article · Mon Apr 02 00:00:00 EDT 2018 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.120.144501· OSTI ID:1505593

Fu, Xiaojing ^[1]; Cueto-Felgueroso, Luis ^[2]; Juanes, Ruben ^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Technical Univ. of Madrid, Madrid (Spain)

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 hydratebearing sediments and other nonequilibrium phenomena commonly observed in natural methane hydrate systems.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FE0013999; SC0018357; FE0013999 and DE-SC0018357

OSTI ID:: 1505593

Alternate ID(s):: OSTI ID: 1430772

Journal Information:: Physical Review Letters, Vol. 120, Issue 14; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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