Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions

Hypothesis: The interfacial free energy between hydrate and water phases is a key thermodynamic parameter that governs both nucleation kinetics and crystal growth of gas hydrates. In these strategic materials—crystalline inclusion compounds where hydrogen-bonded water cages encapsulate small guest m...

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Detalles Bibliográficos
Autores: Zerón, Iván M., Míguez Díaz, José Manuel, Algaba Fernández, Jesús, Mendiboure, Bruno, Jiménez Blas, Felipe
Tipo de recurso: artículo
Fecha de publicación:2026
País:España
Institución:Universidad de Huelva (UHU)
Repositorio:Arias Montano. Repositorio Institucional de la Universidad de Huelva
Idioma:inglés
OAI Identifier:oai:ariasmontano.uhu.es:10272/27989
Acceso en línea:https://hdl.handle.net/10272/27989
Access Level:acceso abierto
Palabra clave:Interfacial free energy
Methane hydrate
Hydrate-water interface
Computer simulation
2210 Química Física
2211 Física del Estado Sólido
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spelling Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditionsZerón, Iván M.Míguez Díaz, José ManuelAlgaba Fernández, JesúsMendiboure, BrunoJiménez Blas, FelipeInterfacial free energyMethane hydrateHydrate-water interfaceComputer simulation2210 Química Física2211 Física del Estado SólidoHypothesis: The interfacial free energy between hydrate and water phases is a key thermodynamic parameter that governs both nucleation kinetics and crystal growth of gas hydrates. In these strategic materials—crystalline inclusion compounds where hydrogen-bonded water cages encapsulate small guest molecules such as methane (CH4) and carbon dioxide (CO2) -this interfacial energy plays a crucial role in determining phase stability and formation pathways. Given the significance of gas hydrates in energy storage, CO2 sequestration, and climate-related processes, accurately determining their interfacial energies is essential for advancing both fundamental understanding and technological applications. Despite its importance, the hydrate–water interfacial energy remains poorly constrained due to substantial experimental uncertainties and the limitations of indirect estimation methods. For example, reported experimental values for CH4 hydrate span a wide range from 28 to 40 mJ/m2. Interestingly, some studies suggest these values are comparable to the interfacial free energy of the hexagonal ice (ice Ih)--water interface, approximately 32 mJ/m2, hinting at potential analogies between clathrate hydrate and ice interfaces. Calculations: In this work, we present a direct molecular simulation of the CH4 hydrate–water interfacial free energy using two novel and independent extensions of the mold integration method. These extensions are specifically designed to induce the formation of a thin, planar hydrate–water interface and to compute the reversible work required to create it. For this purpose, we employ the TIP4P/Ice force field—one of the most reliable water models available—known for accurately reproducing the melting temperature of ice Ih under ambient conditions.Elsevier20262026-01-0120262026-01-01journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/10272/27989reponame:Arias Montano. Repositorio Institucional de la Universidad de Huelvainstname:Universidad de Huelva (UHU)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:ariasmontano.uhu.es:10272/279892026-06-02T14:58:11Z
dc.title.none.fl_str_mv Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions
title Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions
spellingShingle Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions
Zerón, Iván M.
Interfacial free energy
Methane hydrate
Hydrate-water interface
Computer simulation
2210 Química Física
2211 Física del Estado Sólido
title_short Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions
title_full Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions
title_fullStr Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions
title_full_unstemmed Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions
title_sort Unveiling the methane hydrate–water interfacial free energy through direct molecular simulation at coexistence conditions
dc.creator.none.fl_str_mv Zerón, Iván M.
Míguez Díaz, José Manuel
Algaba Fernández, Jesús
Mendiboure, Bruno
Jiménez Blas, Felipe
author Zerón, Iván M.
author_facet Zerón, Iván M.
Míguez Díaz, José Manuel
Algaba Fernández, Jesús
Mendiboure, Bruno
Jiménez Blas, Felipe
author_role author
author2 Míguez Díaz, José Manuel
Algaba Fernández, Jesús
Mendiboure, Bruno
Jiménez Blas, Felipe
author2_role author
author
author
author
dc.contributor.none.fl_str_mv
dc.subject.none.fl_str_mv Interfacial free energy
Methane hydrate
Hydrate-water interface
Computer simulation
2210 Química Física
2211 Física del Estado Sólido
topic Interfacial free energy
Methane hydrate
Hydrate-water interface
Computer simulation
2210 Química Física
2211 Física del Estado Sólido
description Hypothesis: The interfacial free energy between hydrate and water phases is a key thermodynamic parameter that governs both nucleation kinetics and crystal growth of gas hydrates. In these strategic materials—crystalline inclusion compounds where hydrogen-bonded water cages encapsulate small guest molecules such as methane (CH4) and carbon dioxide (CO2) -this interfacial energy plays a crucial role in determining phase stability and formation pathways. Given the significance of gas hydrates in energy storage, CO2 sequestration, and climate-related processes, accurately determining their interfacial energies is essential for advancing both fundamental understanding and technological applications. Despite its importance, the hydrate–water interfacial energy remains poorly constrained due to substantial experimental uncertainties and the limitations of indirect estimation methods. For example, reported experimental values for CH4 hydrate span a wide range from 28 to 40 mJ/m2. Interestingly, some studies suggest these values are comparable to the interfacial free energy of the hexagonal ice (ice Ih)--water interface, approximately 32 mJ/m2, hinting at potential analogies between clathrate hydrate and ice interfaces. Calculations: In this work, we present a direct molecular simulation of the CH4 hydrate–water interfacial free energy using two novel and independent extensions of the mold integration method. These extensions are specifically designed to induce the formation of a thin, planar hydrate–water interface and to compute the reversible work required to create it. For this purpose, we employ the TIP4P/Ice force field—one of the most reliable water models available—known for accurately reproducing the melting temperature of ice Ih under ambient conditions.
publishDate 2026
dc.date.none.fl_str_mv 2026
2026-01-01
2026
2026-01-01
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/10272/27989
url https://hdl.handle.net/10272/27989
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution-NonCommercial-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution-NonCommercial-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
dc.source.none.fl_str_mv reponame:Arias Montano. Repositorio Institucional de la Universidad de Huelva
instname:Universidad de Huelva (UHU)
instname_str Universidad de Huelva (UHU)
reponame_str Arias Montano. Repositorio Institucional de la Universidad de Huelva
collection Arias Montano. Repositorio Institucional de la Universidad de Huelva
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.812429

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