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dc.contributor.author
Longone, Pablo Jesus  
dc.contributor.author
Martín, Ángel  
dc.contributor.author
Ramirez Pastor, Antonio Jose  
dc.date.available
2023-08-16T15:27:18Z  
dc.date.issued
2022-01  
dc.identifier.citation
Longone, Pablo Jesus; Martín, Ángel; Ramirez Pastor, Antonio Jose; CO2-CH4Exchange Process in Structure i Clathrate Hydrates: Calculations of the Thermodynamic Functions Using a Flexible 2D Lattice-Gas Model and Monte Carlo Simulations; American Chemical Society; Journal of Physical Chemistry B; 126; 4; 1-2022; 878-889  
dc.identifier.issn
1520-6106  
dc.identifier.uri
http://hdl.handle.net/11336/208486  
dc.description.abstract
A two-dimensional lattice-gas model, supplemented by Monte Carlo simulations in the grand canonical ensemble, is applied to study the CO2/CH4 exchange process in sI clathrate hydrates. The coverage dependence of the Helmholtz free energy, chemical potential, entropy, and degree of deformation of the sI structure is given. Two different situations are considered according to the value of the intra- and inter-species' interactions. First, lateral interactions between the guest species and water molecules are introduced by following the well-known Lorentz-Berthelot mixing rules. Second, the study is restricted to an ideal clathrate hydrate, where the lateral interactions are neglected and entropy governs the exchange of CH4 by CO2. In the case of real clathrate hydrates (non-zero lateral interactions), the displacement phenomenon is clearly observed from the behavior of the chemical potential and Helmholtz free energy as functions of coverage. The guest species CO2 has an occupation of more than 80% of the cavities, and therefore displaces the CH4 species. Only 13 to 15% of CH4 remains stagnant in the sI structure. With respect to the degree of deformation, a direct relationship between cell distortion and cell occupancy is observed. Finally, the detailed analysis carried out for the ideal clathrate hydrate allows us to interpret the physical mechanism underlying the exchange process: it is entropy, not energy, that drives the displacement of CH4 by CO2 in sI clathrate hydrates.  
dc.format
application/pdf  
dc.language.iso
eng  
dc.publisher
American Chemical Society  
dc.rights
info:eu-repo/semantics/restrictedAccess  
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/  
dc.subject
EXCHANGE  
dc.subject
SIMULATIONS  
dc.subject
HYDRATES  
dc.subject
ENTROPY  
dc.subject.classification
Física de los Materiales Condensados  
dc.subject.classification
Ciencias Físicas  
dc.subject.classification
CIENCIAS NATURALES Y EXACTAS  
dc.title
CO2-CH4Exchange Process in Structure i Clathrate Hydrates: Calculations of the Thermodynamic Functions Using a Flexible 2D Lattice-Gas Model and Monte Carlo Simulations  
dc.type
info:eu-repo/semantics/article  
dc.type
info:ar-repo/semantics/artículo  
dc.type
info:eu-repo/semantics/publishedVersion  
dc.date.updated
2023-07-07T20:28:30Z  
dc.journal.volume
126  
dc.journal.number
4  
dc.journal.pagination
878-889  
dc.journal.pais
Estados Unidos  
dc.journal.ciudad
Washington  
dc.description.fil
Fil: Longone, Pablo Jesus. Universidad Nacional de San Luis. Facultad de Ciencias Físico Matemáticas y Naturales. Departamento de Física; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich". Universidad Nacional de San Luis. Facultad de Ciencias Físico Matemáticas y Naturales. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich"; Argentina  
dc.description.fil
Fil: Martín, Ángel. Universidad de Valladolid; España  
dc.description.fil
Fil: Ramirez Pastor, Antonio Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich". Universidad Nacional de San Luis. Facultad de Ciencias Físico Matemáticas y Naturales. Instituto de Física Aplicada "Dr. Jorge Andrés Zgrablich"; Argentina. Universidad Nacional de San Luis. Facultad de Ciencias Físico Matemáticas y Naturales. Departamento de Física; Argentina  
dc.journal.title
Journal of Physical Chemistry B  
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpcb.1c08942  
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1021/acs.jpcb.1c08942