Pb(II) binding to humic substances: an equilibrium and spectroscopic study

Autores
Orsetti, Silvia; Marco Brown, Jose Luis; Andrade, Estela M.; Molina, Fernando Víctor
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The binding of Pb(II) to humic acids is studied through an approach combining equilibrium and spectroscopic measurements. The methods employed are potentiometric and fluorometric titrations, fluorescence excitation−emission matrices (EEM) and IR spectroscopy. Potentiometric titration curves are analyzed using the NICA equations and an electrostatic model treating the humic particles as an elastic polyelectrolyte network. EEMs are analyzed using parallel factor analysis, decomposing the signal in its independent components and finding their dependence on Pb(II) activity. Potentiometric results are consistent with bimodal affinity distributions for Pb(II) binding, whereas fluorometric titrations are explained by monomodal distributions. EEM analysis is consistent with three independent components in the humic fluorescence response, which are assigned to moieties with different degree of aromaticity. All three components show a similar quenching behavior upon Pb(II) binding, saturating at relatively low Pb(II) concentrations. This is attributed to metal ion induced aggregation of humic molecules, resulting in the interaction between the aromatic groups responsible for fluorescence; this is also consistent with IR spectroscopy results. The observed behavior is interpreted considering that initial metal binding (observed as strongly binding sites), correspond to bi- or multidentate complexation to carboxylate groups, including binding between groups of different humic molecules, promoting aggregation; further metal ions (observed as weakly binding sites) bind to single ligand groups.
Fil: Orsetti, Silvia. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; Argentina
Fil: Marco Brown, Jose Luis. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; Argentina
Fil: Andrade, Estela M.. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina
Fil: Molina, Fernando Víctor. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; Argentina
Materia
Humic Substances
Metal Binding
Fluorescence
Ir Spectroscopy
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:11336/7885

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spelling Pb(II) binding to humic substances: an equilibrium and spectroscopic studyOrsetti, SilviaMarco Brown, Jose LuisAndrade, Estela M.Molina, Fernando VíctorHumic SubstancesMetal BindingFluorescenceIr Spectroscopyhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The binding of Pb(II) to humic acids is studied through an approach combining equilibrium and spectroscopic measurements. The methods employed are potentiometric and fluorometric titrations, fluorescence excitation−emission matrices (EEM) and IR spectroscopy. Potentiometric titration curves are analyzed using the NICA equations and an electrostatic model treating the humic particles as an elastic polyelectrolyte network. EEMs are analyzed using parallel factor analysis, decomposing the signal in its independent components and finding their dependence on Pb(II) activity. Potentiometric results are consistent with bimodal affinity distributions for Pb(II) binding, whereas fluorometric titrations are explained by monomodal distributions. EEM analysis is consistent with three independent components in the humic fluorescence response, which are assigned to moieties with different degree of aromaticity. All three components show a similar quenching behavior upon Pb(II) binding, saturating at relatively low Pb(II) concentrations. This is attributed to metal ion induced aggregation of humic molecules, resulting in the interaction between the aromatic groups responsible for fluorescence; this is also consistent with IR spectroscopy results. The observed behavior is interpreted considering that initial metal binding (observed as strongly binding sites), correspond to bi- or multidentate complexation to carboxylate groups, including binding between groups of different humic molecules, promoting aggregation; further metal ions (observed as weakly binding sites) bind to single ligand groups.Fil: Orsetti, Silvia. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; ArgentinaFil: Marco Brown, Jose Luis. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; ArgentinaFil: Andrade, Estela M.. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; ArgentinaFil: Molina, Fernando Víctor. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; ArgentinaAmerican Chemical Society2013-06-27info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/7885Orsetti, Silvia; Marco Brown, Jose Luis; Andrade, Estela M.; Molina, Fernando Víctor; Pb(II) binding to humic substances: an equilibrium and spectroscopic study; American Chemical Society; Environmental Science & Technology; 47; 15; 27-6-2013; 8325-83330013-936Xenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/es400999qinfo:eu-repo/semantics/altIdentifier/doi/10.1021/es400999qinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T10:09:40Zoai:ri.conicet.gov.ar:11336/7885instacron: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:34982025-09-03 10:09:40.336CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Pb(II) binding to humic substances: an equilibrium and spectroscopic study
title Pb(II) binding to humic substances: an equilibrium and spectroscopic study
spellingShingle Pb(II) binding to humic substances: an equilibrium and spectroscopic study
Orsetti, Silvia
Humic Substances
Metal Binding
Fluorescence
Ir Spectroscopy
title_short Pb(II) binding to humic substances: an equilibrium and spectroscopic study
title_full Pb(II) binding to humic substances: an equilibrium and spectroscopic study
title_fullStr Pb(II) binding to humic substances: an equilibrium and spectroscopic study
title_full_unstemmed Pb(II) binding to humic substances: an equilibrium and spectroscopic study
title_sort Pb(II) binding to humic substances: an equilibrium and spectroscopic study
dc.creator.none.fl_str_mv Orsetti, Silvia
Marco Brown, Jose Luis
Andrade, Estela M.
Molina, Fernando Víctor
author Orsetti, Silvia
author_facet Orsetti, Silvia
Marco Brown, Jose Luis
Andrade, Estela M.
Molina, Fernando Víctor
author_role author
author2 Marco Brown, Jose Luis
Andrade, Estela M.
Molina, Fernando Víctor
author2_role author
author
author
dc.subject.none.fl_str_mv Humic Substances
Metal Binding
Fluorescence
Ir Spectroscopy
topic Humic Substances
Metal Binding
Fluorescence
Ir Spectroscopy
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The binding of Pb(II) to humic acids is studied through an approach combining equilibrium and spectroscopic measurements. The methods employed are potentiometric and fluorometric titrations, fluorescence excitation−emission matrices (EEM) and IR spectroscopy. Potentiometric titration curves are analyzed using the NICA equations and an electrostatic model treating the humic particles as an elastic polyelectrolyte network. EEMs are analyzed using parallel factor analysis, decomposing the signal in its independent components and finding their dependence on Pb(II) activity. Potentiometric results are consistent with bimodal affinity distributions for Pb(II) binding, whereas fluorometric titrations are explained by monomodal distributions. EEM analysis is consistent with three independent components in the humic fluorescence response, which are assigned to moieties with different degree of aromaticity. All three components show a similar quenching behavior upon Pb(II) binding, saturating at relatively low Pb(II) concentrations. This is attributed to metal ion induced aggregation of humic molecules, resulting in the interaction between the aromatic groups responsible for fluorescence; this is also consistent with IR spectroscopy results. The observed behavior is interpreted considering that initial metal binding (observed as strongly binding sites), correspond to bi- or multidentate complexation to carboxylate groups, including binding between groups of different humic molecules, promoting aggregation; further metal ions (observed as weakly binding sites) bind to single ligand groups.
Fil: Orsetti, Silvia. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; Argentina
Fil: Marco Brown, Jose Luis. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; Argentina
Fil: Andrade, Estela M.. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina
Fil: Molina, Fernando Víctor. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de Los Materiales, Medioambiente y Energía; Argentina. Universidad de Buenos Aires; Argentina
description The binding of Pb(II) to humic acids is studied through an approach combining equilibrium and spectroscopic measurements. The methods employed are potentiometric and fluorometric titrations, fluorescence excitation−emission matrices (EEM) and IR spectroscopy. Potentiometric titration curves are analyzed using the NICA equations and an electrostatic model treating the humic particles as an elastic polyelectrolyte network. EEMs are analyzed using parallel factor analysis, decomposing the signal in its independent components and finding their dependence on Pb(II) activity. Potentiometric results are consistent with bimodal affinity distributions for Pb(II) binding, whereas fluorometric titrations are explained by monomodal distributions. EEM analysis is consistent with three independent components in the humic fluorescence response, which are assigned to moieties with different degree of aromaticity. All three components show a similar quenching behavior upon Pb(II) binding, saturating at relatively low Pb(II) concentrations. This is attributed to metal ion induced aggregation of humic molecules, resulting in the interaction between the aromatic groups responsible for fluorescence; this is also consistent with IR spectroscopy results. The observed behavior is interpreted considering that initial metal binding (observed as strongly binding sites), correspond to bi- or multidentate complexation to carboxylate groups, including binding between groups of different humic molecules, promoting aggregation; further metal ions (observed as weakly binding sites) bind to single ligand groups.
publishDate 2013
dc.date.none.fl_str_mv 2013-06-27
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/11336/7885
Orsetti, Silvia; Marco Brown, Jose Luis; Andrade, Estela M.; Molina, Fernando Víctor; Pb(II) binding to humic substances: an equilibrium and spectroscopic study; American Chemical Society; Environmental Science & Technology; 47; 15; 27-6-2013; 8325-8333
0013-936X
url http://hdl.handle.net/11336/7885
identifier_str_mv Orsetti, Silvia; Marco Brown, Jose Luis; Andrade, Estela M.; Molina, Fernando Víctor; Pb(II) binding to humic substances: an equilibrium and spectroscopic study; American Chemical Society; Environmental Science & Technology; 47; 15; 27-6-2013; 8325-8333
0013-936X
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/es400999q
info:eu-repo/semantics/altIdentifier/doi/10.1021/es400999q
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/
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dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
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instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
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repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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