Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density
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....
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todo:paper_08974756_v27_n3_p808_AndrieuBrunsen2023-10-03T15:43:54Z Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density Andrieu-Brunsen, A. Micoureau, S. Tagliazucchi, M. Szleifer, I. Azzaroni, O. Soler-Illia, G.J.A.A. 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 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. Fil:Tagliazucchi, M. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Soler-Illia, G.J.A.A. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_08974756_v27_n3_p808_AndrieuBrunsen |
| institution |
Universidad de Buenos Aires |
| institution_str |
I-28 |
| repository_str |
R-134 |
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Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) |
| topic |
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 |
| spellingShingle |
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 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 |
| topic_facet |
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 |
| 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. © 2015 American Chemical Society. |
| format |
JOUR |
| author |
Andrieu-Brunsen, A. Micoureau, S. Tagliazucchi, M. Szleifer, I. Azzaroni, O. Soler-Illia, G.J.A.A. |
| author_facet |
Andrieu-Brunsen, A. Micoureau, S. Tagliazucchi, M. Szleifer, I. Azzaroni, O. Soler-Illia, G.J.A.A. |
| author_sort |
Andrieu-Brunsen, A. |
| title |
Mesoporous hybrid thin film membranes with PMETAC@Silica architectures: Controlling ionic gating through the tuning of polyelectrolyte density |
| 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 |
| url |
http://hdl.handle.net/20.500.12110/paper_08974756_v27_n3_p808_AndrieuBrunsen |
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