期刊
CHEMISTRY OF MATERIALS
卷 27, 期 3, 页码 808-821出版社
AMER CHEMICAL SOC
DOI: 10.1021/cm5037953
关键词
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资金
- Landesoffensive zur Entwicklung Wissenschaftlich-okonomischer Exzellenz (LOEWE Soft Control) Agencia Nacional de Promocion Cientifica y Tecnologica (ANPCyT) [PICT 1848, 2087, PAE 2004 22711, PICT 2010-457, PICT-PRH 163/08]
- Centro Interdisciplinario de Nanociencia y Nanotecnologia (CINN) [PAE 2006 37063, PRH 2007-74, 74, PME 00038]
- Fundacion Petruzza, Gabbos [DG-017]
- Max-Planck-Gesellschaft (Max Planck Partner Group - MPIP/INIFTA)
- Consejo Nacional de Investigaciones Cientificas y Tecnicas (CONICET) [PIP 11220100100186]
- Alexander von Humboldt Stiftung
- Laboratorio Nacional de Luz Sincrotron (LNLS) [XRD2-11639/10736, SXS-11642]
- Universidad de Buenos Aires (UBACYT) [20020090100164]
- National Science Foundation of USA [CBET-1403058]
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1403058] Funding Source: National Science Foundation
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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