Abstract:
Rational construction of interfaces based on multicomponent responsive systems in which molecular transport is mediated by structures of nanoscale dimensions has become a very fertile research area in biomimetic supramolecular chemistry. Herein, we describe the creation of hybrid mesostructured interfaces with reversible gate-like transport properties that can be controlled by chemical inputs, such as protons or calcium ions. This was accomplished by taking advantage of the surface-initiated polymerization of 2-(methacryloyloxy) ethyl phosphate (MEP) monomer units into and onto mesoporous silica thin films. In this way, phosphate-bearing polymer brushes were used as " gatekeepers" located not only on the outer surface of mesoporous thin films but also in the inner environment of the porous scaffold. Pore-confined PMEP brushes respond to the external triggering chemical signals not only by altering their physicochemical properties but also by switching the transport properties of the mesoporous film. The ion-gate response/operation was based on the protonation and/or chelation of phosphate monomer units in which the polymer brush works as an off-on switch in response to the presence of protons or Ca 2+ ions. The hybrid meso-architectured interface and their functional features were studied by acombination of experimental techniques including ellipso-porosimetry, cyclic voltammetry, X-ray reflectivity, grazing incidence small-angle X-ray scattering, X-ray photoelectron spectroscopy, and in situ atomic force microscopy. In this context, we believe that the integration of stimuli-responsive polymer brushes into nanoscopic supramolecular architectures would provide new routes toward multifunctional biomimetic nanosystems displaying transport properties similar to those encountered in biological ligand-gated ion channels. © 2012 American Chemical Society.
Registro:
Documento: |
Artículo
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Título: | Proton and calcium-gated ionic mesochannels: Phosphate-bearing polymer brushes hosted in mesoporous thin films as biomimetic interfacial architectures |
Autor: | Brunsen, A.; Díaz, C.; Pietrasanta, L.I.; Yameen, B.; Ceolín, M.; Soler-Illia, G.J.A.A.; Azzaroni, O. |
Filiación: | Gerencia Química, Comisión Nacional de Energía Atómica (CNEA), Argentina Centro de Microscopías Avanzadas, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Argentina Max-Planck-Institut für Polymerforschung, Mainz, Germany Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas (INIFTA), Departamento de Química, CONICET, Argentina Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET), C1033AAJ Buenos Aires, Argentina
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Palabras clave: | Calcium ions; Chemical signals; Experimental techniques; Functional features; Grazing incidence small-angle X-ray scattering; In-situ; Interfacial architecture; Ligand-gated ion channels; Mesochannels; Mesoporous films; Mesoporous silica thin films; Mesoporous thin films; Mesostructured; Molecular transport; Monomer units; Multicomponents; Nanoscale dimensions; Outer surface; Phosphate monomers; Physicochemical property; Polymer brushes; Porous scaffold; Rational construction; Stimuli-responsive polymer; Supramolecular architectures; Surface initiated polymerization; X ray reflectivity; Atomic force microscopy; Biomimetics; Cyclic voltammetry; Ions; Mesoporous materials; Monomers; Nanosystems; Phosphate deposits; Photoelectrons; Protons; Scaffolds; Supramolecular chemistry; Thin films; Transport properties; X ray photoelectron spectroscopy; Functional polymers; biomimetic material; calcium; ligand gated ion channel; nanomaterial; phosphate; polymer; proton; article; artificial membrane; biomimetics; chemistry; methodology; porosity; Biomimetic Materials; Biomimetics; Calcium; Ligand-Gated Ion Channels; Membranes, Artificial; Nanostructures; Phosphates; Polymers; Porosity; Protons |
Año: | 2012
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Volumen: | 28
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Número: | 7
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Página de inicio: | 3583
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Página de fin: | 3592
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DOI: |
http://dx.doi.org/10.1021/la204854r |
Título revista: | Langmuir
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Título revista abreviado: | Langmuir
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ISSN: | 07437463
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CODEN: | LANGD
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CAS: | calcium, 14092-94-5, 7440-70-2; phosphate, 14066-19-4, 14265-44-2; proton, 12408-02-5, 12586-59-3; Calcium, 7440-70-2; Ligand-Gated Ion Channels; Membranes, Artificial; Phosphates; Polymers; Protons
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Registro: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_07437463_v28_n7_p3583_Brunsen |
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Citas:
---------- APA ----------
Brunsen, A., Díaz, C., Pietrasanta, L.I., Yameen, B., Ceolín, M., Soler-Illia, G.J.A.A. & Azzaroni, O.
(2012)
. Proton and calcium-gated ionic mesochannels: Phosphate-bearing polymer brushes hosted in mesoporous thin films as biomimetic interfacial architectures. Langmuir, 28(7), 3583-3592.
http://dx.doi.org/10.1021/la204854r---------- CHICAGO ----------
Brunsen, A., Díaz, C., Pietrasanta, L.I., Yameen, B., Ceolín, M., Soler-Illia, G.J.A.A., et al.
"Proton and calcium-gated ionic mesochannels: Phosphate-bearing polymer brushes hosted in mesoporous thin films as biomimetic interfacial architectures"
. Langmuir 28, no. 7
(2012) : 3583-3592.
http://dx.doi.org/10.1021/la204854r---------- MLA ----------
Brunsen, A., Díaz, C., Pietrasanta, L.I., Yameen, B., Ceolín, M., Soler-Illia, G.J.A.A., et al.
"Proton and calcium-gated ionic mesochannels: Phosphate-bearing polymer brushes hosted in mesoporous thin films as biomimetic interfacial architectures"
. Langmuir, vol. 28, no. 7, 2012, pp. 3583-3592.
http://dx.doi.org/10.1021/la204854r---------- VANCOUVER ----------
Brunsen, A., Díaz, C., Pietrasanta, L.I., Yameen, B., Ceolín, M., Soler-Illia, G.J.A.A., et al. Proton and calcium-gated ionic mesochannels: Phosphate-bearing polymer brushes hosted in mesoporous thin films as biomimetic interfacial architectures. Langmuir. 2012;28(7):3583-3592.
http://dx.doi.org/10.1021/la204854r