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Abstract:

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. © 2015 American Chemical Society.

Registro:

Documento: Artículo
Título:Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
Autor:Andrieu-Brunsen, A.; Micoureau, S.; Tagliazucchi, M.; Szleifer, I.; Azzaroni, O.; Soler-Illia, G.J.A.A.
Filiación:Department of Chemistry, LOEWE Soft Control, Technische Universität Darmstadt, Alarich-Weiss-Str. 4, Darmstadt, 64287, Germany
Gerencia Química, Comisión Nacional de Energía Atomica, Centro Atómico Constituyentes, Avda. Gral. Paz 1499, San Martín, Buenos Aires, B1650KNA, Argentina
Department of Biomedical Engineering, Life Processes Institute, Northwestern University, Evanston, IL 60208, United States
Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas (INIFTA), Departamento de Química, Universidad Nacional de la Plata, CC16, Suc. 4, La Plata, Buenos Aires, Argentina
Departamento de Química Inorgánica, Analítica y Química Física, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Buenos Aires, (C1428EHA), Argentina
Palabras clave:Cyclic voltammetry; Infrared spectroscopy; Mesoporous materials; Polyelectrolytes; Polymerization; Silica; Controlled polymerization; Controlled transport; Hybrid architectures; Mesoporous hybrids; Molecular transport; Polymerization routes; Synthetic membranes; Theoretical calculations; Polymers
Año:2015
Volumen:27
Número:3
Página de inicio:808
Página de fin:821
DOI: http://dx.doi.org/10.1021/cm5037953
Título revista:Chemistry of Materials
Título revista abreviado:Chem. Mater.
ISSN:08974756
CODEN:CMATE
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_08974756_v27_n3_p808_AndrieuBrunsen

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Citas:

---------- APA ----------
Andrieu-Brunsen, A., Micoureau, S., Tagliazucchi, M., Szleifer, I., Azzaroni, O. & Soler-Illia, G.J.A.A. (2015) . Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density. Chemistry of Materials, 27(3), 808-821.
http://dx.doi.org/10.1021/cm5037953
---------- CHICAGO ----------
Andrieu-Brunsen, A., Micoureau, S., Tagliazucchi, M., Szleifer, I., Azzaroni, O., Soler-Illia, G.J.A.A. "Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density" . Chemistry of Materials 27, no. 3 (2015) : 808-821.
http://dx.doi.org/10.1021/cm5037953
---------- MLA ----------
Andrieu-Brunsen, A., Micoureau, S., Tagliazucchi, M., Szleifer, I., Azzaroni, O., Soler-Illia, G.J.A.A. "Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density" . Chemistry of Materials, vol. 27, no. 3, 2015, pp. 808-821.
http://dx.doi.org/10.1021/cm5037953
---------- VANCOUVER ----------
Andrieu-Brunsen, A., Micoureau, S., Tagliazucchi, M., Szleifer, I., Azzaroni, O., Soler-Illia, G.J.A.A. Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density. Chem. Mater. 2015;27(3):808-821.
http://dx.doi.org/10.1021/cm5037953