Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)

Natural waters contain mixtures of ligands, which collectively affect the availability of trace metals. The individual contribution of each complex to the overall metal flux received by a sensor can be described in terms of its lability degree. The question arises as to whether the mixture entails s...

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Autores: Altier Infantes, Alexandra, Jiménez-Piedrahita, Martín, Uribe Kaffure, Ramiro, Rey-Castro, Carlos, Cecilia Averós, Joan, Galceran i Nogués, Josep, Puy Llorens, Jaume
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:10459.1/64774
Acceso en línea:https://doi.org/10.1071/EN17232
http://hdl.handle.net/10459.1/64774
Access Level:acceso abierto
Palabra clave:Lability degree
Diffusion coefficients
Mixture effects
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spelling Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)Altier Infantes, AlexandraJiménez-Piedrahita, MartínUribe Kaffure, RamiroRey-Castro, CarlosCecilia Averós, JoanGalceran i Nogués, JosepPuy Llorens, JaumeLability degreeDiffusion coefficientsMixture effectsNatural waters contain mixtures of ligands, which collectively affect the availability of trace metals. The individual contribution of each complex to the overall metal flux received by a sensor can be described in terms of its lability degree. The question arises as to whether the mixture entails specific non-additive effects, i.e. to what extent is it possible to predict the collective behaviour of the mixture from the values of the lability degree of each single ligand system (SLS). For this reason, a series of experiments with diffusion gradients in thin films (DGT) devices were carried out to measure nickel accumulation from synthetic media comprising either nitrilotriacetic acid (NTA), ethylenediamine (EN) or mixtures of both ligands. The results were compared with numerical simulations. It is shown that NiNTA becomes more inert in the mixture than in the SLS that contains the same concentration of free Ni and NiNTA, whereas the opposite is true for the Ni bound to EN, which becomes more labile in the mixture than in the SLS. This unprecedented behaviour arises when one of the ligands (NTA, forming strong and partially labile complexes) is present under non-excess conditions. As NiNTA and NiEN have an opposite influence on the lability degree of each other, the sum of partial fluxes calculated from the lability degrees obtained in SLSs yields a reasonable estimate of DGT performance in the mixture. Experimental accumulations in the mixture are just slightly below the predicted values, with errors lower than 11 % when NTA concentrations vary from 20 to 100 % of the total Ni concentration.The authors gratefully acknowledge support for this research from the Spanish Ministry of Economy, Industry and Competitiveness MINECO (Project CTM2016-78798). The assistance of Federico Quattrini and Calin A. David is acknowledged.CSIRO Publishing2018info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionhttps://doi.org/10.1071/EN17232http://hdl.handle.net/10459.1/64774reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)Inglésinfo:eu-repo/grantAgreement/MINECO//CTM2016-78798Versió postprint del document publicat a https://doi.org/10.1071/EN17232Environmental Chemistry, 2018, vol. 15, núm. 3, p. 183-193(c) CSIRO, 2018info:eu-repo/semantics/openAccessoai:recercat.cat:10459.1/647742026-05-29T05:05:01Z
dc.title.none.fl_str_mv Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)
title Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)
spellingShingle Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)
Altier Infantes, Alexandra
Lability degree
Diffusion coefficients
Mixture effects
title_short Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)
title_full Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)
title_fullStr Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)
title_full_unstemmed Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)
title_sort Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT)
dc.creator.none.fl_str_mv Altier Infantes, Alexandra
Jiménez-Piedrahita, Martín
Uribe Kaffure, Ramiro
Rey-Castro, Carlos
Cecilia Averós, Joan
Galceran i Nogués, Josep
Puy Llorens, Jaume
author Altier Infantes, Alexandra
author_facet Altier Infantes, Alexandra
Jiménez-Piedrahita, Martín
Uribe Kaffure, Ramiro
Rey-Castro, Carlos
Cecilia Averós, Joan
Galceran i Nogués, Josep
Puy Llorens, Jaume
author_role author
author2 Jiménez-Piedrahita, Martín
Uribe Kaffure, Ramiro
Rey-Castro, Carlos
Cecilia Averós, Joan
Galceran i Nogués, Josep
Puy Llorens, Jaume
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv Lability degree
Diffusion coefficients
Mixture effects
topic Lability degree
Diffusion coefficients
Mixture effects
description Natural waters contain mixtures of ligands, which collectively affect the availability of trace metals. The individual contribution of each complex to the overall metal flux received by a sensor can be described in terms of its lability degree. The question arises as to whether the mixture entails specific non-additive effects, i.e. to what extent is it possible to predict the collective behaviour of the mixture from the values of the lability degree of each single ligand system (SLS). For this reason, a series of experiments with diffusion gradients in thin films (DGT) devices were carried out to measure nickel accumulation from synthetic media comprising either nitrilotriacetic acid (NTA), ethylenediamine (EN) or mixtures of both ligands. The results were compared with numerical simulations. It is shown that NiNTA becomes more inert in the mixture than in the SLS that contains the same concentration of free Ni and NiNTA, whereas the opposite is true for the Ni bound to EN, which becomes more labile in the mixture than in the SLS. This unprecedented behaviour arises when one of the ligands (NTA, forming strong and partially labile complexes) is present under non-excess conditions. As NiNTA and NiEN have an opposite influence on the lability degree of each other, the sum of partial fluxes calculated from the lability degrees obtained in SLSs yields a reasonable estimate of DGT performance in the mixture. Experimental accumulations in the mixture are just slightly below the predicted values, with errors lower than 11 % when NTA concentrations vary from 20 to 100 % of the total Ni concentration.
publishDate 2018
dc.date.none.fl_str_mv 2018
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv https://doi.org/10.1071/EN17232
http://hdl.handle.net/10459.1/64774
url https://doi.org/10.1071/EN17232
http://hdl.handle.net/10459.1/64774
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/MINECO//CTM2016-78798
Versió postprint del document publicat a https://doi.org/10.1071/EN17232
Environmental Chemistry, 2018, vol. 15, núm. 3, p. 183-193
dc.rights.none.fl_str_mv (c) CSIRO, 2018
info:eu-repo/semantics/openAccess
rights_invalid_str_mv (c) CSIRO, 2018
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv CSIRO Publishing
publisher.none.fl_str_mv CSIRO Publishing
dc.source.none.fl_str_mv reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
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repository.mail.fl_str_mv
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