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Abstract:

The design of hybrid mesoporous materials incorporating polymeric assemblies as versatile functional units has become a very fertile research area offering major opportunities for controlling molecular transport through interfaces. However, the creation of such functional materials depends critically on our ability to assemble polymeric units in a predictable manner within mesopores with dimensions comparable to the size of the macromolecular blocks themselves. In this work, we describe for the first time the manipulation of the molecular transport properties of mesoporous silica thin films by the direct infiltration of polyelectrolytes into the inner environment of the 3D porous framework. The hybrid architectures were built up through the infiltration-electrostatic assembly of polyallylamine (PAH) on the mesopore silica walls, and the resulting systems were studied by a combination of experimental techniques including ellipso-porosimetry, cyclic voltammetry and X-ray photoelectron spectroscopy, among others. Our results show that the infiltration-assembly of PAH alters the intrinsic cation-permselective properties of mesoporous silica films, rendering them ion-permeable mesochannels and enabling the unrestricted diffusion of cationic and anionic species through the hybrid interfacial architecture. Contrary to what happens during the electrostatic assembly of PAH on planar silica films (quantitative charge reversal), the surface charge of the mesoporous walls is completely neutralized upon assembling the cationic PAH layer (i.e., no charge reversal occurs). We consider this work to have profound implications not only on the molecular design of multifunctional mesoporous thin films but also on understanding the predominant role of nanoconfinement effects in dictating the functional properties of polymer-inorganic hybrid nanomaterials. © 2011 American Chemical Society.

Registro:

Documento: Artículo
Título:Manipulation of molecular transport into mesoporous silica thin films by the infiltration of polyelectrolytes
Autor:Brunsen, A.; Calvo, A.; Williams, F.J.; Soler-Illia, G.J.A.A.; Azzaroni, O.
Filiación:Gerencia de Química, Comisión Nacional de Energía Atómica (CNEA), Argentina
INQUIMAE, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Argentina
Departamento de Química, Facultad de Ciencias Exactas, Universidad Nacional de la Plata, CONICET, Argentina
Palabras clave:Anionic species; Charge reversal; Electrostatic assembly; Experimental techniques; Functional properties; Functional units; Hybrid architectures; Inorganic hybrids; Interfacial architecture; Meso-pores; Mesochannels; Mesopore; Mesoporous silica film; Mesoporous silica thin films; Mesoporous thin films; Mesoporous walls; Molecular design; Molecular transport; Molecular transport properties; Nanoconfinement effects; Planar silica; Polyallylamine; Polymeric assemblies; Porosimetry; Research areas; Cyclic voltammetry; Dyes; Electrostatics; Functional materials; Functional polymers; Hybrid materials; Polyelectrolytes; Polymer films; Polymers; Seepage; Silica; Soil mechanics; Thin films; Transport properties; Walls (structural partitions); X ray photoelectron spectroscopy; Mesoporous materials; electrolyte; nanomaterial; polymer; silicon dioxide; article; artificial membrane; chemistry; permeability; porosity; Electrolytes; Membranes, Artificial; Nanostructures; Permeability; Polymers; Porosity; Silicon Dioxide
Año:2011
Volumen:27
Número:8
Página de inicio:4328
Página de fin:4333
DOI: http://dx.doi.org/10.1021/la200501h
Título revista:Langmuir
Título revista abreviado:Langmuir
ISSN:07437463
CODEN:LANGD
CAS:silicon dioxide, 10279-57-9, 14464-46-1, 14808-60-7, 15468-32-3, 60676-86-0, 7631-86-9; Electrolytes; Membranes, Artificial; Polymers; Silicon Dioxide, 7631-86-9
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_07437463_v27_n8_p4328_Brunsen

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Citas:

---------- APA ----------
Brunsen, A., Calvo, A., Williams, F.J., Soler-Illia, G.J.A.A. & Azzaroni, O. (2011) . Manipulation of molecular transport into mesoporous silica thin films by the infiltration of polyelectrolytes. Langmuir, 27(8), 4328-4333.
http://dx.doi.org/10.1021/la200501h
---------- CHICAGO ----------
Brunsen, A., Calvo, A., Williams, F.J., Soler-Illia, G.J.A.A., Azzaroni, O. "Manipulation of molecular transport into mesoporous silica thin films by the infiltration of polyelectrolytes" . Langmuir 27, no. 8 (2011) : 4328-4333.
http://dx.doi.org/10.1021/la200501h
---------- MLA ----------
Brunsen, A., Calvo, A., Williams, F.J., Soler-Illia, G.J.A.A., Azzaroni, O. "Manipulation of molecular transport into mesoporous silica thin films by the infiltration of polyelectrolytes" . Langmuir, vol. 27, no. 8, 2011, pp. 4328-4333.
http://dx.doi.org/10.1021/la200501h
---------- VANCOUVER ----------
Brunsen, A., Calvo, A., Williams, F.J., Soler-Illia, G.J.A.A., Azzaroni, O. Manipulation of molecular transport into mesoporous silica thin films by the infiltration of polyelectrolytes. Langmuir. 2011;27(8):4328-4333.
http://dx.doi.org/10.1021/la200501h