Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs

Autores
Serra, Ramiro Marcelo; Miro, Eduardo Ernesto; Bolcatto, Pablo Guillermo; Boix, Alicia Viviana
Año de publicación
2011
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In this work, we studied the adsorption capacity and thermal stability of toluene on ZSM5 and mordenite zeolites with different exchange cations (H, Na and Cs). The interaction of the hydrocarbon molecules with the adsorption sites was also addressed with both experimental and theoretical techniques. Flow-adsorption measurements were carried out in order to obtain breakthrough curves as well as TPD experiments. Molecular simulations were performed using the Density Function Theory (DFT). The results show that, in general, mordenite samples have a better adsorption capacity than ZSM5 samples and that the thermal stability of the adsorbed toluene is more influenced by the exchanged cations than by the zeolite structure. The overall basicity of the samples depends on the exchanged cations, following the Cs > Na > H order. The main interaction of toluene takes place between the π electrons of the aromatic ring and the Lewis sites generated, and another interaction takes place between C?H groups and the zeolite network oxygen. The increase of the Cs loading decreases the surface area and pore volume of the zeolites, thus decreasing the available sites for the overall toluene adsorption at 100 °C. Through TPD experiments both the Φ parameter, which represents the fraction of toluene retained at temperatures higher than 100 °C, and the temperature at which the toluene desorbs were measured. It was observed that in the Cs exchanged samples, Φ is higher but the thermal stability (temperature of the maximum desorption rate on TPD) follows the order NaMOR = NaZSM5 > CsNaZSM5 > CsNaMOR > CsHMOR = CsHZSM5 > HMOR > HZSM5. The molecular calculations for the NaMOR structure determined that the interaction energies were higher for NaMOR when compared with the HMOR structure and increased even more when Cs was exchanged. These facts are in line with the experimental results.
Fil: Serra, Ramiro Marcelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Miro, Eduardo Ernesto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Bolcatto, Pablo Guillermo. Universidad Nacional del Litoral. Facultad de Ingeniería Química. Departamento de Física; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe; Argentina
Fil: Boix, Alicia Viviana. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Materia
adsorption
zeolite
toluene
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:11336/277842
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/277842
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with CsSerra, Ramiro MarceloMiro, Eduardo ErnestoBolcatto, Pablo GuillermoBoix, Alicia Vivianaadsorptionzeolitetoluenehttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1https://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1In this work, we studied the adsorption capacity and thermal stability of toluene on ZSM5 and mordenite zeolites with different exchange cations (H, Na and Cs). The interaction of the hydrocarbon molecules with the adsorption sites was also addressed with both experimental and theoretical techniques. Flow-adsorption measurements were carried out in order to obtain breakthrough curves as well as TPD experiments. Molecular simulations were performed using the Density Function Theory (DFT). The results show that, in general, mordenite samples have a better adsorption capacity than ZSM5 samples and that the thermal stability of the adsorbed toluene is more influenced by the exchanged cations than by the zeolite structure. The overall basicity of the samples depends on the exchanged cations, following the Cs > Na > H order. The main interaction of toluene takes place between the π electrons of the aromatic ring and the Lewis sites generated, and another interaction takes place between C?H groups and the zeolite network oxygen. The increase of the Cs loading decreases the surface area and pore volume of the zeolites, thus decreasing the available sites for the overall toluene adsorption at 100 °C. Through TPD experiments both the Φ parameter, which represents the fraction of toluene retained at temperatures higher than 100 °C, and the temperature at which the toluene desorbs were measured. It was observed that in the Cs exchanged samples, Φ is higher but the thermal stability (temperature of the maximum desorption rate on TPD) follows the order NaMOR = NaZSM5 > CsNaZSM5 > CsNaMOR > CsHMOR = CsHZSM5 > HMOR > HZSM5. The molecular calculations for the NaMOR structure determined that the interaction energies were higher for NaMOR when compared with the HMOR structure and increased even more when Cs was exchanged. These facts are in line with the experimental results.Fil: Serra, Ramiro Marcelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; ArgentinaFil: Miro, Eduardo Ernesto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; ArgentinaFil: Bolcatto, Pablo Guillermo. Universidad Nacional del Litoral. Facultad de Ingeniería Química. Departamento de Física; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe; ArgentinaFil: Boix, Alicia Viviana. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; ArgentinaElsevier Science2011-05info: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/11336/277842Serra, Ramiro Marcelo; Miro, Eduardo Ernesto; Bolcatto, Pablo Guillermo; Boix, Alicia Viviana; Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs; Elsevier Science; Microporous and Mesoporous Materials; 147; 1; 5-2011; 17-291387-1811CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S138718111100237Xinfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.micromeso.2011.05.016info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-12-23T14:45:13Zoai:ri.conicet.gov.ar:11336/277842instacron: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:34982025-12-23 14:45:13.658CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs
title Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs
spellingShingle Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs
Serra, Ramiro Marcelo
adsorption
zeolite
toluene
title_short Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs
title_full Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs
title_fullStr Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs
title_full_unstemmed Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs
title_sort Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs
dc.creator.none.fl_str_mv Serra, Ramiro Marcelo
Miro, Eduardo Ernesto
Bolcatto, Pablo Guillermo
Boix, Alicia Viviana
author Serra, Ramiro Marcelo
author_facet Serra, Ramiro Marcelo
Miro, Eduardo Ernesto
Bolcatto, Pablo Guillermo
Boix, Alicia Viviana
author_role author
author2 Miro, Eduardo Ernesto
Bolcatto, Pablo Guillermo
Boix, Alicia Viviana
author2_role author
author
author
dc.subject.none.fl_str_mv adsorption
zeolite
toluene
topic adsorption
zeolite
toluene
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv In this work, we studied the adsorption capacity and thermal stability of toluene on ZSM5 and mordenite zeolites with different exchange cations (H, Na and Cs). The interaction of the hydrocarbon molecules with the adsorption sites was also addressed with both experimental and theoretical techniques. Flow-adsorption measurements were carried out in order to obtain breakthrough curves as well as TPD experiments. Molecular simulations were performed using the Density Function Theory (DFT). The results show that, in general, mordenite samples have a better adsorption capacity than ZSM5 samples and that the thermal stability of the adsorbed toluene is more influenced by the exchanged cations than by the zeolite structure. The overall basicity of the samples depends on the exchanged cations, following the Cs > Na > H order. The main interaction of toluene takes place between the π electrons of the aromatic ring and the Lewis sites generated, and another interaction takes place between C?H groups and the zeolite network oxygen. The increase of the Cs loading decreases the surface area and pore volume of the zeolites, thus decreasing the available sites for the overall toluene adsorption at 100 °C. Through TPD experiments both the Φ parameter, which represents the fraction of toluene retained at temperatures higher than 100 °C, and the temperature at which the toluene desorbs were measured. It was observed that in the Cs exchanged samples, Φ is higher but the thermal stability (temperature of the maximum desorption rate on TPD) follows the order NaMOR = NaZSM5 > CsNaZSM5 > CsNaMOR > CsHMOR = CsHZSM5 > HMOR > HZSM5. The molecular calculations for the NaMOR structure determined that the interaction energies were higher for NaMOR when compared with the HMOR structure and increased even more when Cs was exchanged. These facts are in line with the experimental results.
Fil: Serra, Ramiro Marcelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Miro, Eduardo Ernesto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Bolcatto, Pablo Guillermo. Universidad Nacional del Litoral. Facultad de Ingeniería Química. Departamento de Física; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe; Argentina
Fil: Boix, Alicia Viviana. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
description In this work, we studied the adsorption capacity and thermal stability of toluene on ZSM5 and mordenite zeolites with different exchange cations (H, Na and Cs). The interaction of the hydrocarbon molecules with the adsorption sites was also addressed with both experimental and theoretical techniques. Flow-adsorption measurements were carried out in order to obtain breakthrough curves as well as TPD experiments. Molecular simulations were performed using the Density Function Theory (DFT). The results show that, in general, mordenite samples have a better adsorption capacity than ZSM5 samples and that the thermal stability of the adsorbed toluene is more influenced by the exchanged cations than by the zeolite structure. The overall basicity of the samples depends on the exchanged cations, following the Cs > Na > H order. The main interaction of toluene takes place between the π electrons of the aromatic ring and the Lewis sites generated, and another interaction takes place between C?H groups and the zeolite network oxygen. The increase of the Cs loading decreases the surface area and pore volume of the zeolites, thus decreasing the available sites for the overall toluene adsorption at 100 °C. Through TPD experiments both the Φ parameter, which represents the fraction of toluene retained at temperatures higher than 100 °C, and the temperature at which the toluene desorbs were measured. It was observed that in the Cs exchanged samples, Φ is higher but the thermal stability (temperature of the maximum desorption rate on TPD) follows the order NaMOR = NaZSM5 > CsNaZSM5 > CsNaMOR > CsHMOR = CsHZSM5 > HMOR > HZSM5. The molecular calculations for the NaMOR structure determined that the interaction energies were higher for NaMOR when compared with the HMOR structure and increased even more when Cs was exchanged. These facts are in line with the experimental results.
publishDate 2011
dc.date.none.fl_str_mv 2011-05
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/11336/277842
Serra, Ramiro Marcelo; Miro, Eduardo Ernesto; Bolcatto, Pablo Guillermo; Boix, Alicia Viviana; Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs; Elsevier Science; Microporous and Mesoporous Materials; 147; 1; 5-2011; 17-29
1387-1811
CONICET Digital
CONICET
url http://hdl.handle.net/11336/277842
identifier_str_mv Serra, Ramiro Marcelo; Miro, Eduardo Ernesto; Bolcatto, Pablo Guillermo; Boix, Alicia Viviana; Experimental and theoretical studies about the adsorption of toluene on ZSM5 and mordenite zeolites modified with Cs; Elsevier Science; Microporous and Mesoporous Materials; 147; 1; 5-2011; 17-29
1387-1811
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S138718111100237X
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.micromeso.2011.05.016
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 12.952241

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