Mesoporous Hybrid Thin Film Membranes with PMETAC@Silica Architectures: Controlling Ionic Gating through the Tuning of Polyelectrolyte Density

Annette Andrieu-Brunsen; Sébastien Micoureau; Mario Tagliazucchi; Igal Szleifer; Omar Azzaroni; Galo J. A. A. Soler-Illia

doi:10.1021/cm5037953

journal article·2015-02-10Open access

Mesoporous Hybrid Thin Film Membranes with PMETAC@Silica Architectures: Controlling Ionic Gating through the Tuning of Polyelectrolyte Density

Annette Andrieu-Brunsen, Sébastien Micoureau, Mario Tagliazucchi, Igal Szleifer, Omar Azzaroni, Galo J. A. A. Soler-Illia

Chemistry of Materials· Volume 27· Issue 3

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Source abstract

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.

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Research context

Polymers

OpenAlex topics: Fuel Cells and Related Materials · Nanopore and Nanochannel Transport Studies · Analytical Chemistry and Sensors

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, LOEWE “Soft Control”, Technische Universität Darmstadt, Alarich-Weiss-Str. 4, 64287 Darmstadt, Germany

Gerencia Química, Comisión Nacional de Energía Atomica, Centro Atómico Constituyentes, Avda. Gral. Paz 1499, B1650KNA, San Martín, Buenos Aires, Argentina

Department of Biomedical Engineering, Department of Chemistry and Chemistry of Life Processes Institute, Northwestern University, Evanston, Illinois 60208, United States

Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas (INIFTA), CONICET, and Departamento de Química, Facultad de Ciencias Exactas, 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, Pabellón 2, Ciudad Universitaria (C1428EHA), Buenos Aires, Argentina

Funding

Ministério da Ciência, Tecnologia e Inovação · Consejo Nacional de Investigaciones Científicas y Técnicas · Agencia Nacional de Promoción Científica y Tecnológica · Max-Planck-Gesellschaft · Hessisches Ministerium für Wissenschaft und Kunst · Centro Interdisciplinario de Nanociencia y Nanotecnologi´a, Universidad Nacional Autónoma de México,Baja California · Fundación Petruzza

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