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

Fu, Xiaojing; Waite, William F.; Cueto‐Felgueroso, Luis; Juanes, Ruben

doi:10.1029/2019gc008250

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

Journal Article · 29 May 2019 · Geochemistry, Geophysics, Geosystems

DOI: https://doi.org/10.1029/2019gc008250 · OSTI ID:1614195

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Univ. of California, Berkeley, CA (United States)
U.S. Geological Survey, Woods Hole, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Technical Univ. of Madrid (Spain)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

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.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); US Geological Survey, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: FE0013999; SC0018357; FE0023495

OSTI ID:: 1614195

Alternate ID(s):: OSTI ID: 1523330

Journal Information:: Geochemistry, Geophysics, Geosystems, Vol. 20, Issue 5; ISSN 1525-2027

Publisher:: American Geophysical UnionCopyright Statement

Country of Publication:: United States

Language:: English

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