Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures

Autores
Zalazar, Maria Fernanda; Cabral, Néstor Damián; Romero Ojeda, Gonzalo D.; Alegre, Clara Iris Aymará; Peruchena, Nelida Maria
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In the present work, we studied the protonation reaction of styrene inside the cavity of acidic H-Y zeolite. Density functional theory calculation using M06-2X functional and analysis of quantum theory of atoms in molecules are used to investigate the confinement effects of zeolite framework on species involved on the reaction. A detailed analysis of the topology of the electron density of interactions among reactants, transition state, and intermediate products with the cavity of H-Y zeolite is performed, extracting conclusions about adsorption, catalysis, and confinement effects. Identification and quantification of host-guest interactions between zeolite framework and styryl cation support the larger contribution of weak closed-shell interactions in stabilization of the formed carbenium ion. Our results clearly show that reaction energies for all formed species inside a zeolite with large void structure are also significantly governed by the confinement effects related to weak host-guest interactions. In other words, zeolite confinement effect is a crucial factor that may affect the catalytic activity even on zeolites with large pore size and void structure as H-Y.
Fil: Zalazar, Maria Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; Argentina. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina
Fil: Cabral, Néstor Damián. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina
Fil: Romero Ojeda, Gonzalo D.. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina
Fil: Alegre, Clara Iris Aymará. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; Argentina
Fil: Peruchena, Nelida Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; Argentina. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina
Materia
Zeolites
Confinement Effects
heterogeneous catalysts
QTAIM
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:11336/130769

id CONICETDig_1980652b4ee15215d86856d250d5dc3a
oai_identifier_str oai:ri.conicet.gov.ar:11336/130769
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void StructuresZalazar, Maria FernandaCabral, Néstor DamiánRomero Ojeda, Gonzalo D.Alegre, Clara Iris AymaráPeruchena, Nelida MariaZeolitesConfinement Effectsheterogeneous catalystsQTAIMhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1In the present work, we studied the protonation reaction of styrene inside the cavity of acidic H-Y zeolite. Density functional theory calculation using M06-2X functional and analysis of quantum theory of atoms in molecules are used to investigate the confinement effects of zeolite framework on species involved on the reaction. A detailed analysis of the topology of the electron density of interactions among reactants, transition state, and intermediate products with the cavity of H-Y zeolite is performed, extracting conclusions about adsorption, catalysis, and confinement effects. Identification and quantification of host-guest interactions between zeolite framework and styryl cation support the larger contribution of weak closed-shell interactions in stabilization of the formed carbenium ion. Our results clearly show that reaction energies for all formed species inside a zeolite with large void structure are also significantly governed by the confinement effects related to weak host-guest interactions. In other words, zeolite confinement effect is a crucial factor that may affect the catalytic activity even on zeolites with large pore size and void structure as H-Y.Fil: Zalazar, Maria Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; Argentina. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; ArgentinaFil: Cabral, Néstor Damián. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; ArgentinaFil: Romero Ojeda, Gonzalo D.. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; ArgentinaFil: Alegre, Clara Iris Aymará. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; ArgentinaFil: Peruchena, Nelida Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; Argentina. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; ArgentinaAmerican Chemical Society2018-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/130769Zalazar, Maria Fernanda; Cabral, Néstor Damián; Romero Ojeda, Gonzalo D.; Alegre, Clara Iris Aymará; Peruchena, Nelida Maria; Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures; American Chemical Society; Journal of Physical Chemistry C; 122; 48; 12-2018; 27350-273591932-7447CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpcc.8b07357info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpcc.8b07357info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:20:44Zoai:ri.conicet.gov.ar:11336/130769instacron: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:34982025-10-22 11:20:44.955CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures
title Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures
spellingShingle Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures
Zalazar, Maria Fernanda
Zeolites
Confinement Effects
heterogeneous catalysts
QTAIM
title_short Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures
title_full Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures
title_fullStr Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures
title_full_unstemmed Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures
title_sort Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures
dc.creator.none.fl_str_mv Zalazar, Maria Fernanda
Cabral, Néstor Damián
Romero Ojeda, Gonzalo D.
Alegre, Clara Iris Aymará
Peruchena, Nelida Maria
author Zalazar, Maria Fernanda
author_facet Zalazar, Maria Fernanda
Cabral, Néstor Damián
Romero Ojeda, Gonzalo D.
Alegre, Clara Iris Aymará
Peruchena, Nelida Maria
author_role author
author2 Cabral, Néstor Damián
Romero Ojeda, Gonzalo D.
Alegre, Clara Iris Aymará
Peruchena, Nelida Maria
author2_role author
author
author
author
dc.subject.none.fl_str_mv Zeolites
Confinement Effects
heterogeneous catalysts
QTAIM
topic Zeolites
Confinement Effects
heterogeneous catalysts
QTAIM
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv In the present work, we studied the protonation reaction of styrene inside the cavity of acidic H-Y zeolite. Density functional theory calculation using M06-2X functional and analysis of quantum theory of atoms in molecules are used to investigate the confinement effects of zeolite framework on species involved on the reaction. A detailed analysis of the topology of the electron density of interactions among reactants, transition state, and intermediate products with the cavity of H-Y zeolite is performed, extracting conclusions about adsorption, catalysis, and confinement effects. Identification and quantification of host-guest interactions between zeolite framework and styryl cation support the larger contribution of weak closed-shell interactions in stabilization of the formed carbenium ion. Our results clearly show that reaction energies for all formed species inside a zeolite with large void structure are also significantly governed by the confinement effects related to weak host-guest interactions. In other words, zeolite confinement effect is a crucial factor that may affect the catalytic activity even on zeolites with large pore size and void structure as H-Y.
Fil: Zalazar, Maria Fernanda. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; Argentina. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina
Fil: Cabral, Néstor Damián. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina
Fil: Romero Ojeda, Gonzalo D.. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina
Fil: Alegre, Clara Iris Aymará. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; Argentina
Fil: Peruchena, Nelida Maria. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Nordeste. Instituto de Química Básica y Aplicada del Nordeste Argentino. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas Naturales y Agrimensura. Instituto de Química Básica y Aplicada del Nordeste Argentino; Argentina. Universidad Nacional del Nordeste. Facultad de Ciencias Exactas y Naturales y Agrimensura. Departamento de Química. Laboratorio de Estructura Molecular y Propiedades; Argentina
description In the present work, we studied the protonation reaction of styrene inside the cavity of acidic H-Y zeolite. Density functional theory calculation using M06-2X functional and analysis of quantum theory of atoms in molecules are used to investigate the confinement effects of zeolite framework on species involved on the reaction. A detailed analysis of the topology of the electron density of interactions among reactants, transition state, and intermediate products with the cavity of H-Y zeolite is performed, extracting conclusions about adsorption, catalysis, and confinement effects. Identification and quantification of host-guest interactions between zeolite framework and styryl cation support the larger contribution of weak closed-shell interactions in stabilization of the formed carbenium ion. Our results clearly show that reaction energies for all formed species inside a zeolite with large void structure are also significantly governed by the confinement effects related to weak host-guest interactions. In other words, zeolite confinement effect is a crucial factor that may affect the catalytic activity even on zeolites with large pore size and void structure as H-Y.
publishDate 2018
dc.date.none.fl_str_mv 2018-12
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/11336/130769
Zalazar, Maria Fernanda; Cabral, Néstor Damián; Romero Ojeda, Gonzalo D.; Alegre, Clara Iris Aymará; Peruchena, Nelida Maria; Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures; American Chemical Society; Journal of Physical Chemistry C; 122; 48; 12-2018; 27350-27359
1932-7447
CONICET Digital
CONICET
url http://hdl.handle.net/11336/130769
identifier_str_mv Zalazar, Maria Fernanda; Cabral, Néstor Damián; Romero Ojeda, Gonzalo D.; Alegre, Clara Iris Aymará; Peruchena, Nelida Maria; Confinement Effects in Protonation Reactions Catalyzed by Zeolites with Large Void Structures; American Chemical Society; Journal of Physical Chemistry C; 122; 48; 12-2018; 27350-27359
1932-7447
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpcc.8b07357
info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpcc.8b07357
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
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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
_version_ 1846781701881069568
score 12.8982525