Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption

Autores
Dávila, M.; Romá, Federico José; Riccardo, Jose Luis; Ramirez Pastor, Antonio Jose
Año de publicación
2006
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The statistical thermodynamics of interacting polyatomic adsorbates (k-mers) on homogeneous surfaces was developed on a generalization in the spirit of the lattice-gas model and the quasi-chemical approximation (QCA). The new theoretical framework is obtained by combining (i) the exact analytical expression for the partition function of non-interacting linear k-mers adsorbed in one dimension and its extension to higher dimensions, and (ii) a generalization of the classical QCA in which the adsorbate can occupy more than one adsorption site. The coverage and temperature dependence of the Helmholtz free energy, chemical potential, configurational entropy, configurational energy, isosteric heat of adsorption and specific heat are given. The formalism reproduces the classical QCA for monomers, leads to the exact statistical thermodynamics of interacting k-mers adsorbed in one dimension, and provides a close approximation for two-dimensional systems accounting multisite occupancy. Comparisons with analytical data from Bragg-Williams approximation (BWA) and Monte Carlo simulations are performed in order to test the validity of the theoretical model. The resulting thermodynamic description is significantly better than the BWA and still mathematically handable.
Fil: Dávila, M.. Universidad Nacional de San Luis; Argentina. Comisión Nacional de Energía Atómica. Gerencia del Área de Energía Nuclear. Instituto Balseiro. Archivo Histórico del Centro Atómico Bariloche e Instituto Balseiro | Universidad Nacional de Cuyo. Instituto Balseiro. Archivo Histórico del Centro Atómico Bariloche e Instituto Balseiro; Argentina
Fil: Romá, Federico José. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; Argentina
Fil: Riccardo, Jose Luis. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; Argentina
Fil: Ramirez Pastor, Antonio Jose. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; Argentina
Materia
LATTICE-GAS MODELS
MULTISITE OCCUPANCY
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/214214
Acceder
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network_name_str CONICET Digital (CONICET)
spelling Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorptionDávila, M.Romá, Federico JoséRiccardo, Jose LuisRamirez Pastor, Antonio JoseLATTICE-GAS MODELSMULTISITE OCCUPANCYhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The statistical thermodynamics of interacting polyatomic adsorbates (k-mers) on homogeneous surfaces was developed on a generalization in the spirit of the lattice-gas model and the quasi-chemical approximation (QCA). The new theoretical framework is obtained by combining (i) the exact analytical expression for the partition function of non-interacting linear k-mers adsorbed in one dimension and its extension to higher dimensions, and (ii) a generalization of the classical QCA in which the adsorbate can occupy more than one adsorption site. The coverage and temperature dependence of the Helmholtz free energy, chemical potential, configurational entropy, configurational energy, isosteric heat of adsorption and specific heat are given. The formalism reproduces the classical QCA for monomers, leads to the exact statistical thermodynamics of interacting k-mers adsorbed in one dimension, and provides a close approximation for two-dimensional systems accounting multisite occupancy. Comparisons with analytical data from Bragg-Williams approximation (BWA) and Monte Carlo simulations are performed in order to test the validity of the theoretical model. The resulting thermodynamic description is significantly better than the BWA and still mathematically handable.Fil: Dávila, M.. Universidad Nacional de San Luis; Argentina. Comisión Nacional de Energía Atómica. Gerencia del Área de Energía Nuclear. Instituto Balseiro. Archivo Histórico del Centro Atómico Bariloche e Instituto Balseiro | Universidad Nacional de Cuyo. Instituto Balseiro. Archivo Histórico del Centro Atómico Bariloche e Instituto Balseiro; ArgentinaFil: Romá, Federico José. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; ArgentinaFil: Riccardo, Jose Luis. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; ArgentinaFil: Ramirez Pastor, Antonio Jose. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; ArgentinaElsevier Science2006-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/214214Dávila, M.; Romá, Federico José; Riccardo, Jose Luis; Ramirez Pastor, Antonio Jose; Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption; Elsevier Science; Surface Science; 600; 10; 12-2006; 2011-20250039-6028CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.susc.2006.02.032info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0039602806002184info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:41:03Zoai:ri.conicet.gov.ar:11336/214214instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-29 10:41:03.521CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption
title Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption
spellingShingle Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption
Dávila, M.
LATTICE-GAS MODELS
MULTISITE OCCUPANCY
title_short Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption
title_full Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption
title_fullStr Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption
title_full_unstemmed Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption
title_sort Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption
dc.creator.none.fl_str_mv Dávila, M.
Romá, Federico José
Riccardo, Jose Luis
Ramirez Pastor, Antonio Jose
author Dávila, M.
author_facet Dávila, M.
Romá, Federico José
Riccardo, Jose Luis
Ramirez Pastor, Antonio Jose
author_role author
author2 Romá, Federico José
Riccardo, Jose Luis
Ramirez Pastor, Antonio Jose
author2_role author
author
author
dc.subject.none.fl_str_mv LATTICE-GAS MODELS
MULTISITE OCCUPANCY
topic LATTICE-GAS MODELS
MULTISITE OCCUPANCY
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The statistical thermodynamics of interacting polyatomic adsorbates (k-mers) on homogeneous surfaces was developed on a generalization in the spirit of the lattice-gas model and the quasi-chemical approximation (QCA). The new theoretical framework is obtained by combining (i) the exact analytical expression for the partition function of non-interacting linear k-mers adsorbed in one dimension and its extension to higher dimensions, and (ii) a generalization of the classical QCA in which the adsorbate can occupy more than one adsorption site. The coverage and temperature dependence of the Helmholtz free energy, chemical potential, configurational entropy, configurational energy, isosteric heat of adsorption and specific heat are given. The formalism reproduces the classical QCA for monomers, leads to the exact statistical thermodynamics of interacting k-mers adsorbed in one dimension, and provides a close approximation for two-dimensional systems accounting multisite occupancy. Comparisons with analytical data from Bragg-Williams approximation (BWA) and Monte Carlo simulations are performed in order to test the validity of the theoretical model. The resulting thermodynamic description is significantly better than the BWA and still mathematically handable.
Fil: Dávila, M.. Universidad Nacional de San Luis; Argentina. Comisión Nacional de Energía Atómica. Gerencia del Área de Energía Nuclear. Instituto Balseiro. Archivo Histórico del Centro Atómico Bariloche e Instituto Balseiro | Universidad Nacional de Cuyo. Instituto Balseiro. Archivo Histórico del Centro Atómico Bariloche e Instituto Balseiro; Argentina
Fil: Romá, Federico José. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; Argentina
Fil: Riccardo, Jose Luis. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; Argentina
Fil: Ramirez Pastor, Antonio Jose. Universidad Nacional de San Luis; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis; Argentina
description The statistical thermodynamics of interacting polyatomic adsorbates (k-mers) on homogeneous surfaces was developed on a generalization in the spirit of the lattice-gas model and the quasi-chemical approximation (QCA). The new theoretical framework is obtained by combining (i) the exact analytical expression for the partition function of non-interacting linear k-mers adsorbed in one dimension and its extension to higher dimensions, and (ii) a generalization of the classical QCA in which the adsorbate can occupy more than one adsorption site. The coverage and temperature dependence of the Helmholtz free energy, chemical potential, configurational entropy, configurational energy, isosteric heat of adsorption and specific heat are given. The formalism reproduces the classical QCA for monomers, leads to the exact statistical thermodynamics of interacting k-mers adsorbed in one dimension, and provides a close approximation for two-dimensional systems accounting multisite occupancy. Comparisons with analytical data from Bragg-Williams approximation (BWA) and Monte Carlo simulations are performed in order to test the validity of the theoretical model. The resulting thermodynamic description is significantly better than the BWA and still mathematically handable.
publishDate 2006
dc.date.none.fl_str_mv 2006-12
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/214214
Dávila, M.; Romá, Federico José; Riccardo, Jose Luis; Ramirez Pastor, Antonio Jose; Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption; Elsevier Science; Surface Science; 600; 10; 12-2006; 2011-2025
0039-6028
CONICET Digital
CONICET
url http://hdl.handle.net/11336/214214
identifier_str_mv Dávila, M.; Romá, Federico José; Riccardo, Jose Luis; Ramirez Pastor, Antonio Jose; Quasi-chemical approximation for polyatomics: Statistical thermodynamics of adsorption; Elsevier Science; Surface Science; 600; 10; 12-2006; 2011-2025
0039-6028
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.susc.2006.02.032
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0039602806002184
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science
publisher.none.fl_str_mv Elsevier Science
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.070432

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