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Xenon Hydrate as an Analog of Methane Hydrate in Geologic Systems Out of Thermodynamic Equilibrium

Fu, Xiaojing and Waite, William F. and Cueto‐Felgueroso, Luis and Juanes, Ruben (2019) Xenon Hydrate as an Analog of Methane Hydrate in Geologic Systems Out of Thermodynamic Equilibrium. Geochemistry, Geophysics, Geosystems, 20 (5). pp. 2462-2472. ISSN 1525-2027. https://resolver.caltech.edu/CaltechAUTHORS:20200902-134918986

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Abstract

Methane hydrate occurs naturally under pressure and temperature conditions that are not straightforward to replicate experimentally. Xenon has emerged as an attractive laboratory alternative to methane for studying hydrate formation and dissociation in multiphase systems, given that it forms hydrates under milder conditions. However, building reliable analogies between the two hydrates requires systematic comparisons, which are currently lacking. We address this gap by developing a theoretical and computational model of gas hydrates under equilibrium and nonequilibrium conditions. We first compare equilibrium phase behaviors of the Xe·H₂O and CH₄·H₂O systems by calculating their isobaric phase diagram, and then study the nonequilibrium kinetics of interfacial hydrate growth using a phase field model. Our results show that Xe·H₂O is a good experimental analog to CH₄·H₂O, but there are key differences to consider. In particular, the aqueous solubility of xenon is altered by the presence of hydrate, similar to what is observed for methane; but xenon is consistently less soluble than methane. Xenon hydrate has a wider nonstoichiometry region, which could lead to a thicker hydrate layer at the gas‐liquid interface when grown under similar kinetic forcing conditions. For both systems, our numerical calculations reveal that hydrate nonstoichiometry coupled with hydrate formation dynamics leads to a compositional gradient across the hydrate layer, where the stoichiometric ratio increases from the gas‐facing side to the liquid‐facing side. Our analysis suggests that accurate composition measurements could be used to infer the kinetic history of hydrate formation in natural settings where gas is abundant.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1029/2019gc008250DOIArticle
https://doi.org/10.6078/D1G67BDOIData
ORCID:
AuthorORCID
Fu, Xiaojing0000-0001-7120-704X
Waite, William F.0000-0002-9436-4109
Cueto‐Felgueroso, Luis0000-0001-5303-0236
Juanes, Ruben0000-0002-7370-2332
Additional Information:© 2019 American Geophysical Union. Issue Online: 14 June 2019; Version of Record online: 29 May 2019; Accepted manuscript online: 06 May 2019; Manuscript accepted: 23 April 2019; Manuscript revised: 15 April 2019; Manuscript received: 31 January 2019. This work was funded in part by the U.S. Department of Energy, DOE [awards DE‐FE0013999 and DE‐SC0018357 (to R. J.) and DOE Interagency Agreement DE‐FE0023495 (to W. F. W.)]. X. F. acknowledges support by the Miller Research Fellowship at the University of California Berkeley. W. F. W. acknowledges support from the U.S. Geological Survey's Gas Hydrate Project and the Survey's Coastal, Marine Hazards and Resources Program. L. C. F. acknowledges funding from the Spanish Ministry of Economy and Competitiveness (grants RYC‐2012‐11704 and CTM2014‐54312‐P). L. C. F. and R. J. acknowledge funding from the MIT International Science and Technology Initiatives, through a Seed Fund grant. The simulation data are available on the UC Berkeley Dash repository at https://doi.org/10.6078/D1G67B.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE‐FE0013999
Department of Energy (DOE)DE‐SC0018357
Department of Energy (DOE)DE‐FE0023495
Miller Institute for Basic Research in ScienceUNSPECIFIED
USGSUNSPECIFIED
Ministerio de Economía, Industria y Competitividad (MINECO)RYC‐2012‐11704
Ministerio de Economía, Industria y Competitividad (MINECO)CTM2014‐54312‐P
Subject Keywords:methane hydrates; xenon hydrates; phase behavior; growth kinetics; nonstoichiometry
Issue or Number:5
Record Number:CaltechAUTHORS:20200902-134918986
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200902-134918986
Official Citation:Fu, X., Waite, W. F., Cueto‐Felgueroso, L., & Juanes, R. (2019). Xenon hydrate as an analog of methane hydrate in geologic systems out of thermodynamic equilibrium. Geochemistry, Geophysics, Geosystems, 20, 2462–2472. https://doi.org/10.1029/2019GC008250
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:105222
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:08 Sep 2020 23:49
Last Modified:08 Sep 2020 23:49

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