Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films

Autores
Pérez Chávez, Néstor Ariel; Albesa, Alberto Gustavo; Longo, Gabriel Sebastian
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A molecular theory has been applied to study the equilibrium conditions of glyphosate and aminomethylphosphonic acid (AMPA) adsorption from aqueous solutions to hydrogel films of cross-linked polyallylamine (PAH). This theoretical framework allows for describing the size, shape, state of charge/protonation, and configurational freedom of all chemical species in the system. Adsorption of glyphosate is a nonmonotonic function of the solution pH, which results from the protonation behavior of both the adsorbate and adsorbent material. Glyphosate and chloride ions compete for adsorption to neutralize the polymer charge; lowering the solution salt concentration enhances the partition of glyphosate inside the hydrogel film. AMPA adsorption is qualitatively similar to that of glyphosate but orders of magnitude smaller under the same conditions. AMPA is less charged than glyphosate, which unbalances the competition for adsorption with salt counter ions. In mixed solutions, glyphosate presence can significantly hinder AMPA adsorption. A higher pH establishes inside the film than in the bulk solution, which has important implications for the herbicide biodegradation because microbial activity is pH-dependent. Thus, PAH hydrogel films can be considered as functional materials that combine glyphosate sequestration and in situ degradation. In devising these materials, the polymer density is an important variable of design; polymer networks with high density of titratable units can enhance adsorption; this density can also be used to modify the pH inside the material.
Fil: Pérez Chávez, Néstor Ariel. 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: Albesa, Alberto Gustavo. 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: Longo, Gabriel Sebastian. 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
pH-RESPONSIVE HYDROGELS
GLYPHOSATE SEQUESTRATION
MOLECULAR SIMULATIONS
POLY(ALLYLAMINE) FILMS
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:11336/100827
Acceder
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network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine FilmsPérez Chávez, Néstor ArielAlbesa, Alberto GustavoLongo, Gabriel SebastianpH-RESPONSIVE HYDROGELSGLYPHOSATE SEQUESTRATIONMOLECULAR SIMULATIONSPOLY(ALLYLAMINE) FILMShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1A molecular theory has been applied to study the equilibrium conditions of glyphosate and aminomethylphosphonic acid (AMPA) adsorption from aqueous solutions to hydrogel films of cross-linked polyallylamine (PAH). This theoretical framework allows for describing the size, shape, state of charge/protonation, and configurational freedom of all chemical species in the system. Adsorption of glyphosate is a nonmonotonic function of the solution pH, which results from the protonation behavior of both the adsorbate and adsorbent material. Glyphosate and chloride ions compete for adsorption to neutralize the polymer charge; lowering the solution salt concentration enhances the partition of glyphosate inside the hydrogel film. AMPA adsorption is qualitatively similar to that of glyphosate but orders of magnitude smaller under the same conditions. AMPA is less charged than glyphosate, which unbalances the competition for adsorption with salt counter ions. In mixed solutions, glyphosate presence can significantly hinder AMPA adsorption. A higher pH establishes inside the film than in the bulk solution, which has important implications for the herbicide biodegradation because microbial activity is pH-dependent. Thus, PAH hydrogel films can be considered as functional materials that combine glyphosate sequestration and in situ degradation. In devising these materials, the polymer density is an important variable of design; polymer networks with high density of titratable units can enhance adsorption; this density can also be used to modify the pH inside the material.Fil: Pérez Chávez, Néstor Ariel. 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: Albesa, Alberto Gustavo. 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: Longo, Gabriel Sebastian. 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 Society2018-10info: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/11336/100827Pérez Chávez, Néstor Ariel; Albesa, Alberto Gustavo; Longo, Gabriel Sebastian; Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films; American Chemical Society; Langmuir; 34; 42; 10-2018; 12560-125680743-7463CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/10.1021/acs.langmuir.8b02727info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.langmuir.8b02727info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.langmuir.8b02727info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:09:44Zoai:ri.conicet.gov.ar:11336/100827instacron: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:34982025-10-22 11:09:44.547CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films
title Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films
spellingShingle Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films
Pérez Chávez, Néstor Ariel
pH-RESPONSIVE HYDROGELS
GLYPHOSATE SEQUESTRATION
MOLECULAR SIMULATIONS
POLY(ALLYLAMINE) FILMS
title_short Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films
title_full Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films
title_fullStr Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films
title_full_unstemmed Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films
title_sort Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films
dc.creator.none.fl_str_mv Pérez Chávez, Néstor Ariel
Albesa, Alberto Gustavo
Longo, Gabriel Sebastian
author Pérez Chávez, Néstor Ariel
author_facet Pérez Chávez, Néstor Ariel
Albesa, Alberto Gustavo
Longo, Gabriel Sebastian
author_role author
author2 Albesa, Alberto Gustavo
Longo, Gabriel Sebastian
author2_role author
author
dc.subject.none.fl_str_mv pH-RESPONSIVE HYDROGELS
GLYPHOSATE SEQUESTRATION
MOLECULAR SIMULATIONS
POLY(ALLYLAMINE) FILMS
topic pH-RESPONSIVE HYDROGELS
GLYPHOSATE SEQUESTRATION
MOLECULAR SIMULATIONS
POLY(ALLYLAMINE) FILMS
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv A molecular theory has been applied to study the equilibrium conditions of glyphosate and aminomethylphosphonic acid (AMPA) adsorption from aqueous solutions to hydrogel films of cross-linked polyallylamine (PAH). This theoretical framework allows for describing the size, shape, state of charge/protonation, and configurational freedom of all chemical species in the system. Adsorption of glyphosate is a nonmonotonic function of the solution pH, which results from the protonation behavior of both the adsorbate and adsorbent material. Glyphosate and chloride ions compete for adsorption to neutralize the polymer charge; lowering the solution salt concentration enhances the partition of glyphosate inside the hydrogel film. AMPA adsorption is qualitatively similar to that of glyphosate but orders of magnitude smaller under the same conditions. AMPA is less charged than glyphosate, which unbalances the competition for adsorption with salt counter ions. In mixed solutions, glyphosate presence can significantly hinder AMPA adsorption. A higher pH establishes inside the film than in the bulk solution, which has important implications for the herbicide biodegradation because microbial activity is pH-dependent. Thus, PAH hydrogel films can be considered as functional materials that combine glyphosate sequestration and in situ degradation. In devising these materials, the polymer density is an important variable of design; polymer networks with high density of titratable units can enhance adsorption; this density can also be used to modify the pH inside the material.
Fil: Pérez Chávez, Néstor Ariel. 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: Albesa, Alberto Gustavo. 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: Longo, Gabriel Sebastian. 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 A molecular theory has been applied to study the equilibrium conditions of glyphosate and aminomethylphosphonic acid (AMPA) adsorption from aqueous solutions to hydrogel films of cross-linked polyallylamine (PAH). This theoretical framework allows for describing the size, shape, state of charge/protonation, and configurational freedom of all chemical species in the system. Adsorption of glyphosate is a nonmonotonic function of the solution pH, which results from the protonation behavior of both the adsorbate and adsorbent material. Glyphosate and chloride ions compete for adsorption to neutralize the polymer charge; lowering the solution salt concentration enhances the partition of glyphosate inside the hydrogel film. AMPA adsorption is qualitatively similar to that of glyphosate but orders of magnitude smaller under the same conditions. AMPA is less charged than glyphosate, which unbalances the competition for adsorption with salt counter ions. In mixed solutions, glyphosate presence can significantly hinder AMPA adsorption. A higher pH establishes inside the film than in the bulk solution, which has important implications for the herbicide biodegradation because microbial activity is pH-dependent. Thus, PAH hydrogel films can be considered as functional materials that combine glyphosate sequestration and in situ degradation. In devising these materials, the polymer density is an important variable of design; polymer networks with high density of titratable units can enhance adsorption; this density can also be used to modify the pH inside the material.
publishDate 2018
dc.date.none.fl_str_mv 2018-10
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/11336/100827
Pérez Chávez, Néstor Ariel; Albesa, Alberto Gustavo; Longo, Gabriel Sebastian; Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films; American Chemical Society; Langmuir; 34; 42; 10-2018; 12560-12568
0743-7463
CONICET Digital
CONICET
url http://hdl.handle.net/11336/100827
identifier_str_mv Pérez Chávez, Néstor Ariel; Albesa, Alberto Gustavo; Longo, Gabriel Sebastian; Using Polymer Hydrogels for Glyphosate Sequestration from Aqueous Solutions: Molecular Theory Study of Adsorption to Polyallylamine Films; American Chemical Society; Langmuir; 34; 42; 10-2018; 12560-12568
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/10.1021/acs.langmuir.8b02727
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.langmuir.8b02727
info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.langmuir.8b02727
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 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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