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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/37978
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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 Técnicas2025-09-29T09:48:00Zoai: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:34982025-09-29 09:48:01.277CONICET 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 |
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CONICET Digital (CONICET) |
collection |
CONICET Digital (CONICET) |
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Consejo Nacional de Investigaciones Científicas y Técnicas |
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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 |