Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density

Autores
Andrieu Brunsen, Annette; Micoureau, Sébastien; Tagliazucchi, Mario Eugenio; Szleifer, Igal; Azzaroni, Omar; Soler Illia, Galo Juan de Avila Arturo
Año de publicación
2015
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Manipulating molecular transport through mesoporous hybrid films is a fascinating approach toward mimicking transport in nature. To understand the details in controlled transport, it is necessary to gradually adjust the charge density that in turn results in a precise adjustment of permselectivity. We have created hybrid architectures through the controlled polymerization of a strong polyelectrolyte: (2-methacryloyloxy)ethyltrimethylammounium (PMETAC) in a mesoporous thin silica film. PMETAC contents from 5 to 100% filling can be obtained by choosing a temperature or light-induced polymerization route and by varying polymerization times, as proven by ellipsoporosimetry and infrared spectroscopy. Using cyclic voltammetry, we demonstrate that a gradual variation of ionic permselectivity from a silanol-regulated to a PMETAC-regulated permselectivity can be obtained by tuning the PMETAC mesopore filling. The resulting behavior ranges from ion exclusion to preconcentration. The experimental observations are correlated with theoretical calculations that provide quantitative insights into the organization of the ions and polymers within the pore. Our findings shed light into the understanding of the interplay between charge density and space on molecular transport, leading toward the rational design of selectively transporting synthetic membranes.
Fil: Andrieu Brunsen, Annette. Universitat Technische Darmstadt; Alemania. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Micoureau, Sébastien. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Tagliazucchi, Mario Eugenio. Northwestern University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Szleifer, Igal. Northwestern University; Estados Unidos
Fil: Azzaroni, Omar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Soler Illia, Galo Juan de Avila Arturo. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Materia
Mesoporous Materials
Polyelectrolyte
Molecular Theory
Ion Transport
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:11336/37978
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/37978
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network_name_str CONICET Digital (CONICET)
spelling Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte densityAndrieu Brunsen, AnnetteMicoureau, SébastienTagliazucchi, Mario EugenioSzleifer, IgalAzzaroni, OmarSoler Illia, Galo Juan de Avila ArturoMesoporous MaterialsPolyelectrolyteMolecular TheoryIon Transporthttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Manipulating molecular transport through mesoporous hybrid films is a fascinating approach toward mimicking transport in nature. To understand the details in controlled transport, it is necessary to gradually adjust the charge density that in turn results in a precise adjustment of permselectivity. We have created hybrid architectures through the controlled polymerization of a strong polyelectrolyte: (2-methacryloyloxy)ethyltrimethylammounium (PMETAC) in a mesoporous thin silica film. PMETAC contents from 5 to 100% filling can be obtained by choosing a temperature or light-induced polymerization route and by varying polymerization times, as proven by ellipsoporosimetry and infrared spectroscopy. Using cyclic voltammetry, we demonstrate that a gradual variation of ionic permselectivity from a silanol-regulated to a PMETAC-regulated permselectivity can be obtained by tuning the PMETAC mesopore filling. The resulting behavior ranges from ion exclusion to preconcentration. The experimental observations are correlated with theoretical calculations that provide quantitative insights into the organization of the ions and polymers within the pore. Our findings shed light into the understanding of the interplay between charge density and space on molecular transport, leading toward the rational design of selectively transporting synthetic membranes.Fil: Andrieu Brunsen, Annette. Universitat Technische Darmstadt; Alemania. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; ArgentinaFil: Micoureau, Sébastien. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; ArgentinaFil: Tagliazucchi, Mario Eugenio. Northwestern University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Szleifer, Igal. Northwestern University; Estados UnidosFil: Azzaroni, Omar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaFil: Soler Illia, Galo Juan de Avila Arturo. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaAmerican Chemical Society2015-02info: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/11336/37978Andrieu Brunsen, Annette; Micoureau, Sébastien; Tagliazucchi, Mario Eugenio; Szleifer, Igal; Azzaroni, Omar; et al.; Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density; American Chemical Society; Chemistry Of Materials; 27; 3; 2-2015; 808-8210897-4756CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/cm5037953info:eu-repo/semantics/altIdentifier/doi/10.1021/cm5037953info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:16:51Zoai:ri.conicet.gov.ar:11336/37978instacron: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 11:16:52.176CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
title Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
spellingShingle Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
Andrieu Brunsen, Annette
Mesoporous Materials
Polyelectrolyte
Molecular Theory
Ion Transport
title_short Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
title_full Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
title_fullStr Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
title_full_unstemmed Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
title_sort Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
dc.creator.none.fl_str_mv Andrieu Brunsen, Annette
Micoureau, Sébastien
Tagliazucchi, Mario Eugenio
Szleifer, Igal
Azzaroni, Omar
Soler Illia, Galo Juan de Avila Arturo
author Andrieu Brunsen, Annette
author_facet Andrieu Brunsen, Annette
Micoureau, Sébastien
Tagliazucchi, Mario Eugenio
Szleifer, Igal
Azzaroni, Omar
Soler Illia, Galo Juan de Avila Arturo
author_role author
author2 Micoureau, Sébastien
Tagliazucchi, Mario Eugenio
Szleifer, Igal
Azzaroni, Omar
Soler Illia, Galo Juan de Avila Arturo
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Mesoporous Materials
Polyelectrolyte
Molecular Theory
Ion Transport
topic Mesoporous Materials
Polyelectrolyte
Molecular Theory
Ion Transport
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Manipulating molecular transport through mesoporous hybrid films is a fascinating approach toward mimicking transport in nature. To understand the details in controlled transport, it is necessary to gradually adjust the charge density that in turn results in a precise adjustment of permselectivity. We have created hybrid architectures through the controlled polymerization of a strong polyelectrolyte: (2-methacryloyloxy)ethyltrimethylammounium (PMETAC) in a mesoporous thin silica film. PMETAC contents from 5 to 100% filling can be obtained by choosing a temperature or light-induced polymerization route and by varying polymerization times, as proven by ellipsoporosimetry and infrared spectroscopy. Using cyclic voltammetry, we demonstrate that a gradual variation of ionic permselectivity from a silanol-regulated to a PMETAC-regulated permselectivity can be obtained by tuning the PMETAC mesopore filling. The resulting behavior ranges from ion exclusion to preconcentration. The experimental observations are correlated with theoretical calculations that provide quantitative insights into the organization of the ions and polymers within the pore. Our findings shed light into the understanding of the interplay between charge density and space on molecular transport, leading toward the rational design of selectively transporting synthetic membranes.
Fil: Andrieu Brunsen, Annette. Universitat Technische Darmstadt; Alemania. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Micoureau, Sébastien. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Tagliazucchi, Mario Eugenio. Northwestern University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Szleifer, Igal. Northwestern University; Estados Unidos
Fil: Azzaroni, Omar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Soler Illia, Galo Juan de Avila Arturo. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
description Manipulating molecular transport through mesoporous hybrid films is a fascinating approach toward mimicking transport in nature. To understand the details in controlled transport, it is necessary to gradually adjust the charge density that in turn results in a precise adjustment of permselectivity. We have created hybrid architectures through the controlled polymerization of a strong polyelectrolyte: (2-methacryloyloxy)ethyltrimethylammounium (PMETAC) in a mesoporous thin silica film. PMETAC contents from 5 to 100% filling can be obtained by choosing a temperature or light-induced polymerization route and by varying polymerization times, as proven by ellipsoporosimetry and infrared spectroscopy. Using cyclic voltammetry, we demonstrate that a gradual variation of ionic permselectivity from a silanol-regulated to a PMETAC-regulated permselectivity can be obtained by tuning the PMETAC mesopore filling. The resulting behavior ranges from ion exclusion to preconcentration. The experimental observations are correlated with theoretical calculations that provide quantitative insights into the organization of the ions and polymers within the pore. Our findings shed light into the understanding of the interplay between charge density and space on molecular transport, leading toward the rational design of selectively transporting synthetic membranes.
publishDate 2015
dc.date.none.fl_str_mv 2015-02
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/11336/37978
Andrieu Brunsen, Annette; Micoureau, Sébastien; Tagliazucchi, Mario Eugenio; Szleifer, Igal; Azzaroni, Omar; et al.; Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density; American Chemical Society; Chemistry Of Materials; 27; 3; 2-2015; 808-821
0897-4756
CONICET Digital
CONICET
url http://hdl.handle.net/11336/37978
identifier_str_mv Andrieu Brunsen, Annette; Micoureau, Sébastien; Tagliazucchi, Mario Eugenio; Szleifer, Igal; Azzaroni, Omar; et al.; Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density; American Chemical Society; Chemistry Of Materials; 27; 3; 2-2015; 808-821
0897-4756
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://pubs.acs.org/doi/abs/10.1021/cm5037953
info:eu-repo/semantics/altIdentifier/doi/10.1021/cm5037953
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
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score 12.982451

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