Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures

Autores
Brunsen, Annette; Diaz, Carolina; Pietrasanta, Lia; Yameen, Basit; Ceolin, Marcelo Raul; Soler Illia, Galo Juan de Avila Arturo; Azzaroni, Omar
Año de publicación
2012
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
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 Ca2+ ions. The hybrid meso-architectured interface and their functional features were studied by a combination 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.
Fil: Brunsen, Annette. Comisión Nacional de Energía Atómica. Gerencia del Área de Seguridad Nuclear y Ambiente. Gerencia de Química (CAC); Argentina
Fil: Diaz, Carolina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Pietrasanta, Lia. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Centro de Microscopías Avanzadas; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Yameen, Basit. Max-Planck-Institut fü r Polymerforschung; Alemania
Fil: Ceolin, Marcelo Raul. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Soler Illia, Galo Juan de Avila Arturo. Comisión Nacional de Energía Atómica. Gerencia del Área de Seguridad Nuclear y Ambiente. Gerencia de Química (CAC); Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Azzaroni, Omar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Materia
Ionic channels
Polymer brushes
Mesoporous thin films
Biomimetic interfacial arquitectures
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/273879
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/273879
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial ArchitecturesBrunsen, AnnetteDiaz, CarolinaPietrasanta, LiaYameen, BasitCeolin, Marcelo RaulSoler Illia, Galo Juan de Avila ArturoAzzaroni, OmarIonic channelsPolymer brushesMesoporous thin filmsBiomimetic interfacial arquitectureshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Rational 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 Ca2+ ions. The hybrid meso-architectured interface and their functional features were studied by a combination 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.Fil: Brunsen, Annette. Comisión Nacional de Energía Atómica. Gerencia del Área de Seguridad Nuclear y Ambiente. Gerencia de Química (CAC); ArgentinaFil: Diaz, Carolina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaFil: Pietrasanta, Lia. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Centro de Microscopías Avanzadas; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Yameen, Basit. Max-Planck-Institut fü r Polymerforschung; AlemaniaFil: Ceolin, Marcelo Raul. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaFil: Soler Illia, Galo Juan de Avila Arturo. Comisión Nacional de Energía Atómica. Gerencia del Área de Seguridad Nuclear y Ambiente. Gerencia de Química (CAC); Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Azzaroni, Omar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaAmerican Chemical Society2012-02info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/273879Brunsen, Annette; Diaz, Carolina; Pietrasanta, Lia; Yameen, Basit; Ceolin, Marcelo Raul; et al.; Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures; American Chemical Society; Langmuir; 28; 7; 2-2012; 3583-35920743-7463CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/la204854rinfo:eu-repo/semantics/altIdentifier/doi/10.1021/la204854rinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-11-26T08:47:17Zoai:ri.conicet.gov.ar:11336/273879instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-11-26 08:47:17.282CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures
title Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures
spellingShingle Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures
Brunsen, Annette
Ionic channels
Polymer brushes
Mesoporous thin films
Biomimetic interfacial arquitectures
title_short Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures
title_full Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures
title_fullStr Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures
title_full_unstemmed Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures
title_sort Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures
dc.creator.none.fl_str_mv Brunsen, Annette
Diaz, Carolina
Pietrasanta, Lia
Yameen, Basit
Ceolin, Marcelo Raul
Soler Illia, Galo Juan de Avila Arturo
Azzaroni, Omar
author Brunsen, Annette
author_facet Brunsen, Annette
Diaz, Carolina
Pietrasanta, Lia
Yameen, Basit
Ceolin, Marcelo Raul
Soler Illia, Galo Juan de Avila Arturo
Azzaroni, Omar
author_role author
author2 Diaz, Carolina
Pietrasanta, Lia
Yameen, Basit
Ceolin, Marcelo Raul
Soler Illia, Galo Juan de Avila Arturo
Azzaroni, Omar
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv Ionic channels
Polymer brushes
Mesoporous thin films
Biomimetic interfacial arquitectures
topic Ionic channels
Polymer brushes
Mesoporous thin films
Biomimetic interfacial arquitectures
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv 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 Ca2+ ions. The hybrid meso-architectured interface and their functional features were studied by a combination 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.
Fil: Brunsen, Annette. Comisión Nacional de Energía Atómica. Gerencia del Área de Seguridad Nuclear y Ambiente. Gerencia de Química (CAC); Argentina
Fil: Diaz, Carolina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Pietrasanta, Lia. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Centro de Microscopías Avanzadas; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Yameen, Basit. Max-Planck-Institut fü r Polymerforschung; Alemania
Fil: Ceolin, Marcelo Raul. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Soler Illia, Galo Juan de Avila Arturo. Comisión Nacional de Energía Atómica. Gerencia del Área de Seguridad Nuclear y Ambiente. Gerencia de Química (CAC); Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Azzaroni, Omar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
description 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 Ca2+ ions. The hybrid meso-architectured interface and their functional features were studied by a combination 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.
publishDate 2012
dc.date.none.fl_str_mv 2012-02
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/273879
Brunsen, Annette; Diaz, Carolina; Pietrasanta, Lia; Yameen, Basit; Ceolin, Marcelo Raul; et al.; Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures; American Chemical Society; Langmuir; 28; 7; 2-2012; 3583-3592
0743-7463
CONICET Digital
CONICET
url http://hdl.handle.net/11336/273879
identifier_str_mv Brunsen, Annette; Diaz, Carolina; Pietrasanta, Lia; Yameen, Basit; Ceolin, Marcelo Raul; et al.; Proton and Calcium-Gated Ionic Mesochannels: Phosphate-Bearing Polymer Brushes Hosted in Mesoporous Thin Films As Biomimetic Interfacial Architectures; American Chemical Society; Langmuir; 28; 7; 2-2012; 3583-3592
0743-7463
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/la204854r
info:eu-repo/semantics/altIdentifier/doi/10.1021/la204854r
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.011256

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