Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation

In this work, we determine the dissociation temperature of hydrogen (H2) hydrate by computer simulation using two different methods. In both cases, the molecules of water and H2 are modeled using the TIP4P/Ice and a modified version of the Silvera and Goldman models, respectively, and the Berthelot...

Descripción completa

Detalles Bibliográficos
Autores: Torrejón Ríos, Miguel Jesús, Blázquez, Samuel, Algaba Fernández, Jesús, Martín Conde, María, Jiménez Blas, Felipe
Tipo de recurso: artículo
Fecha de publicación:2025
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:10272/27526
Acceso en línea:https://hdl.handle.net/10272/27526
Access Level:acceso abierto
Palabra clave:2307 Química Física
3312 Tecnología de Materiales
id ES_f4d0fcdff0f37833078e2b2aad4922f7
oai_identifier_str oai:ariasmontano.uhu.es:10272/27526
network_acronym_str ES
network_name_str España
repository_id_str
spelling Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer SimulationTorrejón Ríos, Miguel JesúsBlázquez, SamuelAlgaba Fernández, JesúsMartín Conde, MaríaJiménez Blas, Felipe2307 Química Física3312 Tecnología de MaterialesIn this work, we determine the dissociation temperature of hydrogen (H2) hydrate by computer simulation using two different methods. In both cases, the molecules of water and H2 are modeled using the TIP4P/Ice and a modified version of the Silvera and Goldman models, respectively, and the Berthelot combining rule for the cross water–H2 interactions has been modified. The first method used in this work is the solubility method, which consists of determining the solubility of H2 in an aqueous phase when in contact with the H2 hydrate (H–Lw) phase and when in contact with the pure H2 phase (Lw–LH2) at different temperatures. At a given pressure value, both solubility curves intersect at the temperature (T3) at which the three phases coexist in equilibrium. Following this approach, we determine the dissociation temperature of H2 hydrate at 185 MPa finding a good agreement with the data previously reported in the literature. We also analyze the effect of the multiple occupancy of the D, or small, and H, or large, cages of the sII hydrate structure. We conclude that the T3 value is barely affected by the occupancy of the H2 hydrate at 185 MPa. From the analysis of the solubility curves and performing extra bulk simulations of the three phases involved in the equilibrium, we also determine the driving force for nucleation (ΔμNEC) at 185 MPa as a function of the supercooling degree and the H2 hydrate occupancy. We determine that, thermodynamically, the most favored occupancy of the H2 hydrate consists of 1 H2 molecule in the D cages and 3 in the H cages (i.e., 1–3 occupancy). We also conclude that the double occupancy of the small D cages is not favored because the ΔμNEC values obtained for this occupancy are the most positive ones. The second approach used in this work is the direct coexistence technique using an initial H2 hydrate phase with 1–3 occupancy. We also propose a new modification of the Berthelot combining rule to improve the predictions of the T3 values. Following this method, we determine the T3 at 100, 185, and 300 MPa finding excellent agreement with the experimental data.American Chemical Society20252025-01-0120252025-01-01journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/10272/27526reponame:Arias Montano. Repositorio Institucional de la Universidad de Huelvainstname:Universidad de Huelva (UHU)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution 4.0 Internationalhttp://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:ariasmontano.uhu.es:10272/275262026-06-02T14:58:11Z
dc.title.none.fl_str_mv Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation
title Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation
spellingShingle Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation
Torrejón Ríos, Miguel Jesús
2307 Química Física
3312 Tecnología de Materiales
title_short Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation
title_full Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation
title_fullStr Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation
title_full_unstemmed Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation
title_sort Dissociation Line and Driving Force for Nucleation of the Multiple Occupied Hydrogen Hydrate from Computer Simulation
dc.creator.none.fl_str_mv Torrejón Ríos, Miguel Jesús
Blázquez, Samuel
Algaba Fernández, Jesús
Martín Conde, María
Jiménez Blas, Felipe
author Torrejón Ríos, Miguel Jesús
author_facet Torrejón Ríos, Miguel Jesús
Blázquez, Samuel
Algaba Fernández, Jesús
Martín Conde, María
Jiménez Blas, Felipe
author_role author
author2 Blázquez, Samuel
Algaba Fernández, Jesús
Martín Conde, María
Jiménez Blas, Felipe
author2_role author
author
author
author
dc.contributor.none.fl_str_mv
dc.subject.none.fl_str_mv 2307 Química Física
3312 Tecnología de Materiales
topic 2307 Química Física
3312 Tecnología de Materiales
description In this work, we determine the dissociation temperature of hydrogen (H2) hydrate by computer simulation using two different methods. In both cases, the molecules of water and H2 are modeled using the TIP4P/Ice and a modified version of the Silvera and Goldman models, respectively, and the Berthelot combining rule for the cross water–H2 interactions has been modified. The first method used in this work is the solubility method, which consists of determining the solubility of H2 in an aqueous phase when in contact with the H2 hydrate (H–Lw) phase and when in contact with the pure H2 phase (Lw–LH2) at different temperatures. At a given pressure value, both solubility curves intersect at the temperature (T3) at which the three phases coexist in equilibrium. Following this approach, we determine the dissociation temperature of H2 hydrate at 185 MPa finding a good agreement with the data previously reported in the literature. We also analyze the effect of the multiple occupancy of the D, or small, and H, or large, cages of the sII hydrate structure. We conclude that the T3 value is barely affected by the occupancy of the H2 hydrate at 185 MPa. From the analysis of the solubility curves and performing extra bulk simulations of the three phases involved in the equilibrium, we also determine the driving force for nucleation (ΔμNEC) at 185 MPa as a function of the supercooling degree and the H2 hydrate occupancy. We determine that, thermodynamically, the most favored occupancy of the H2 hydrate consists of 1 H2 molecule in the D cages and 3 in the H cages (i.e., 1–3 occupancy). We also conclude that the double occupancy of the small D cages is not favored because the ΔμNEC values obtained for this occupancy are the most positive ones. The second approach used in this work is the direct coexistence technique using an initial H2 hydrate phase with 1–3 occupancy. We also propose a new modification of the Berthelot combining rule to improve the predictions of the T3 values. Following this method, we determine the T3 at 100, 185, and 300 MPa finding excellent agreement with the experimental data.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025-01-01
2025
2025-01-01
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/10272/27526
url https://hdl.handle.net/10272/27526
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 4.0 International
http://creativecommons.org/licenses/by/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 4.0 International
http://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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
_version_ 1869424506550878208
score 15,812455

Similares en LA Referencia