Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing
- Autores
- Debais, Gabriel; Tagliazucchi, Mario Eugenio
- Año de publicación
- 2020
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- This work applies a molecular theory to study the formation of lateral self-assembled aggregates in mixed brushes composed of polyanion and polycation chains. In order to overcome the well-known limitations of mean-field electrostatics to capture polyelectrolyte complexation, the formation of ion pairs between anionic and cationic groups in the polyelectrolytes is explicitly modeled in our theory as an association reaction. This feature is essential to capture the microphase separation of the mixed brush and the formation of lateral aggregates triggered by polyelectrolyte complexation. The effects of solution pH and ionic strength, surface coverage, and chain length on the morphology of the mixed brush are systematically explored. It is shown that increasing salt concentration leads to the rupture of polyelectrolyte complexes and the stabilization of the homogeneous, non-aggregated brush, providing that the formation of ion pairs between the polyelectrolytes and the salt ions in solution is explicitly accounted for by the theory. The inclusion of ion-pairing association reactions between oppositely charged polyelectrolytes within a mean-field description of electrostatics emerges from this work as a useful and simple theoretical approach to capture the formation of polyelectrolyte complexes and their responsiveness to solution ionic strength and pH.
Fil: Debais, Gabriel. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Tagliazucchi, Mario Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina - Materia
-
Molecular theory
Brush
Ion pair
Self-assembly - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
- Repositorio
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/142582
Ver los metadatos del registro completo
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Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairingDebais, GabrielTagliazucchi, Mario EugenioMolecular theoryBrushIon pairSelf-assemblyhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1This work applies a molecular theory to study the formation of lateral self-assembled aggregates in mixed brushes composed of polyanion and polycation chains. In order to overcome the well-known limitations of mean-field electrostatics to capture polyelectrolyte complexation, the formation of ion pairs between anionic and cationic groups in the polyelectrolytes is explicitly modeled in our theory as an association reaction. This feature is essential to capture the microphase separation of the mixed brush and the formation of lateral aggregates triggered by polyelectrolyte complexation. The effects of solution pH and ionic strength, surface coverage, and chain length on the morphology of the mixed brush are systematically explored. It is shown that increasing salt concentration leads to the rupture of polyelectrolyte complexes and the stabilization of the homogeneous, non-aggregated brush, providing that the formation of ion pairs between the polyelectrolytes and the salt ions in solution is explicitly accounted for by the theory. The inclusion of ion-pairing association reactions between oppositely charged polyelectrolytes within a mean-field description of electrostatics emerges from this work as a useful and simple theoretical approach to capture the formation of polyelectrolyte complexes and their responsiveness to solution ionic strength and pH.Fil: Debais, Gabriel. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Tagliazucchi, Mario Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaAmerican Institute of Physics2020-10info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/142582Debais, Gabriel; Tagliazucchi, Mario Eugenio; Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing; American Institute of Physics; Journal of Chemical Physics; 153; 14; 10-2020; 1-130021-9606CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://aip.scitation.org/doi/10.1063/5.0020779info:eu-repo/semantics/altIdentifier/doi/10.1063/5.0020779info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:47:52Zoai:ri.conicet.gov.ar:11336/142582instacron: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:34982025-09-29 09:47:52.429CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing |
title |
Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing |
spellingShingle |
Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing Debais, Gabriel Molecular theory Brush Ion pair Self-assembly |
title_short |
Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing |
title_full |
Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing |
title_fullStr |
Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing |
title_full_unstemmed |
Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing |
title_sort |
Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing |
dc.creator.none.fl_str_mv |
Debais, Gabriel Tagliazucchi, Mario Eugenio |
author |
Debais, Gabriel |
author_facet |
Debais, Gabriel Tagliazucchi, Mario Eugenio |
author_role |
author |
author2 |
Tagliazucchi, Mario Eugenio |
author2_role |
author |
dc.subject.none.fl_str_mv |
Molecular theory Brush Ion pair Self-assembly |
topic |
Molecular theory Brush Ion pair Self-assembly |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
dc.description.none.fl_txt_mv |
This work applies a molecular theory to study the formation of lateral self-assembled aggregates in mixed brushes composed of polyanion and polycation chains. In order to overcome the well-known limitations of mean-field electrostatics to capture polyelectrolyte complexation, the formation of ion pairs between anionic and cationic groups in the polyelectrolytes is explicitly modeled in our theory as an association reaction. This feature is essential to capture the microphase separation of the mixed brush and the formation of lateral aggregates triggered by polyelectrolyte complexation. The effects of solution pH and ionic strength, surface coverage, and chain length on the morphology of the mixed brush are systematically explored. It is shown that increasing salt concentration leads to the rupture of polyelectrolyte complexes and the stabilization of the homogeneous, non-aggregated brush, providing that the formation of ion pairs between the polyelectrolytes and the salt ions in solution is explicitly accounted for by the theory. The inclusion of ion-pairing association reactions between oppositely charged polyelectrolytes within a mean-field description of electrostatics emerges from this work as a useful and simple theoretical approach to capture the formation of polyelectrolyte complexes and their responsiveness to solution ionic strength and pH. Fil: Debais, Gabriel. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina Fil: Tagliazucchi, Mario Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina |
description |
This work applies a molecular theory to study the formation of lateral self-assembled aggregates in mixed brushes composed of polyanion and polycation chains. In order to overcome the well-known limitations of mean-field electrostatics to capture polyelectrolyte complexation, the formation of ion pairs between anionic and cationic groups in the polyelectrolytes is explicitly modeled in our theory as an association reaction. This feature is essential to capture the microphase separation of the mixed brush and the formation of lateral aggregates triggered by polyelectrolyte complexation. The effects of solution pH and ionic strength, surface coverage, and chain length on the morphology of the mixed brush are systematically explored. It is shown that increasing salt concentration leads to the rupture of polyelectrolyte complexes and the stabilization of the homogeneous, non-aggregated brush, providing that the formation of ion pairs between the polyelectrolytes and the salt ions in solution is explicitly accounted for by the theory. The inclusion of ion-pairing association reactions between oppositely charged polyelectrolytes within a mean-field description of electrostatics emerges from this work as a useful and simple theoretical approach to capture the formation of polyelectrolyte complexes and their responsiveness to solution ionic strength and pH. |
publishDate |
2020 |
dc.date.none.fl_str_mv |
2020-10 |
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/11336/142582 Debais, Gabriel; Tagliazucchi, Mario Eugenio; Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing; American Institute of Physics; Journal of Chemical Physics; 153; 14; 10-2020; 1-13 0021-9606 CONICET Digital CONICET |
url |
http://hdl.handle.net/11336/142582 |
identifier_str_mv |
Debais, Gabriel; Tagliazucchi, Mario Eugenio; Microphase separation and aggregate self-assembly in brushes of oppositely charged polyelectrolytes triggered by ion pairing; American Institute of Physics; Journal of Chemical Physics; 153; 14; 10-2020; 1-13 0021-9606 CONICET Digital CONICET |
dc.language.none.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
info:eu-repo/semantics/altIdentifier/url/https://aip.scitation.org/doi/10.1063/5.0020779 info:eu-repo/semantics/altIdentifier/doi/10.1063/5.0020779 |
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 |
dc.publisher.none.fl_str_mv |
American Institute of Physics |
publisher.none.fl_str_mv |
American Institute of Physics |
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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1844613490662178816 |
score |
13.070432 |