A dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices
International audience The speciation of metal species extracted by diffusion gradient in thin films (DGT) devices during experimental deployments in simple metal-ligand synthetic solutions was numerically modeled, analyzed at steady state, and simulated in the dynamic regime. The modeled speciation...
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Online Access: | https://hal.inrae.fr/hal-02581397 https://doi.org/10.1021/es025839o |
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ftccsdartic:oai:HAL:hal-02581397v1 2023-05-15T16:01:50+02:00 A dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices Tusseau-Vuillemin, M.H. Gilbin, R. Taillefert, M. Qualité et fonctionnement hydrologique des systèmes aquatiques (UR QHAN) Centre national du machinisme agricole, du génie rural, des eaux et forêts (CEMAGREF) GEOGIA INSTITUTE OF TECHNOLOGY ATLANTA USA Partenaires IRSTEA Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA) 2003 https://hal.inrae.fr/hal-02581397 https://doi.org/10.1021/es025839o en eng HAL CCSD American Chemical Society info:eu-repo/semantics/altIdentifier/doi/10.1021/es025839o hal-02581397 https://hal.inrae.fr/hal-02581397 doi:10.1021/es025839o IRSTEA: PUB00011571 ISSN: 0013-936X EISSN: 1520-5851 Environmental Science and Technology https://hal.inrae.fr/hal-02581397 Environmental Science and Technology, American Chemical Society, 2003, 37 (8), pp.1645-1652. ⟨10.1021/es025839o⟩ CEMAGREF QHAN [SDE]Environmental Sciences info:eu-repo/semantics/article Journal articles 2003 ftccsdartic https://doi.org/10.1021/es025839o 2022-01-01T23:29:31Z International audience The speciation of metal species extracted by diffusion gradient in thin films (DGT) devices during experimental deployments in simple metal-ligand synthetic solutions was numerically modeled, analyzed at steady state, and simulated in the dynamic regime. The modeled speciation of two well-known complexes (Cu-citrate and Cu-EDTA) are in good agreement with experimental data obtained in NaNO3 solutions. For any metal complex, the rate at which the metal accumulates on the chelating resin is proportional to the concentration of free metal in solution plus a fraction of the metal complex concentration in solution equivalent to zetaD(ML)/D-M. D-M and D-ML are the diffusion coefficients of the free and metal complex, respectively, and zeta characterizes the complex lability: it is defined as the fraction of metal complex lost when diffusing from the bulk solution to the chelating resin. Numerical simulations were used to explore the variations of zeta as a function of several operational and chemical parameters. Lability increases when the dissociation rate constant or the residence time of the metal complex within the hydrogel increase (i.e., by either increasing the thickness of the hydrogel or decreasing DML). Overall, the fraction of metal complex extracted by the DGT decreases when DML decreases, which confirms the ability of diffusion-restrictive hydrogels to separate the free metal fraction from complex solutions. Although the DGT model does not exactly comply with the voltammetric formalism, the lability criteria ATtau(1/2) used with voltammetric macroelectrodes is similar to the lability criteria zeta, except that it is valid for high metal ligand ratio. To determine free metal concentrations in aquatic systems using DGT, it is necessary to account for the presence of numerous ligands with different complexing properties. Soon, the numerical model will be improved to include additional ligands competing for the metal, and new experiments will be designed to discriminate between ... Article in Journal/Newspaper DML Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) Environmental Science & Technology 37 8 1645 1652 |
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Open Polar |
collection |
Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) |
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ftccsdartic |
language |
English |
topic |
CEMAGREF QHAN [SDE]Environmental Sciences |
spellingShingle |
CEMAGREF QHAN [SDE]Environmental Sciences Tusseau-Vuillemin, M.H. Gilbin, R. Taillefert, M. A dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices |
topic_facet |
CEMAGREF QHAN [SDE]Environmental Sciences |
description |
International audience The speciation of metal species extracted by diffusion gradient in thin films (DGT) devices during experimental deployments in simple metal-ligand synthetic solutions was numerically modeled, analyzed at steady state, and simulated in the dynamic regime. The modeled speciation of two well-known complexes (Cu-citrate and Cu-EDTA) are in good agreement with experimental data obtained in NaNO3 solutions. For any metal complex, the rate at which the metal accumulates on the chelating resin is proportional to the concentration of free metal in solution plus a fraction of the metal complex concentration in solution equivalent to zetaD(ML)/D-M. D-M and D-ML are the diffusion coefficients of the free and metal complex, respectively, and zeta characterizes the complex lability: it is defined as the fraction of metal complex lost when diffusing from the bulk solution to the chelating resin. Numerical simulations were used to explore the variations of zeta as a function of several operational and chemical parameters. Lability increases when the dissociation rate constant or the residence time of the metal complex within the hydrogel increase (i.e., by either increasing the thickness of the hydrogel or decreasing DML). Overall, the fraction of metal complex extracted by the DGT decreases when DML decreases, which confirms the ability of diffusion-restrictive hydrogels to separate the free metal fraction from complex solutions. Although the DGT model does not exactly comply with the voltammetric formalism, the lability criteria ATtau(1/2) used with voltammetric macroelectrodes is similar to the lability criteria zeta, except that it is valid for high metal ligand ratio. To determine free metal concentrations in aquatic systems using DGT, it is necessary to account for the presence of numerous ligands with different complexing properties. Soon, the numerical model will be improved to include additional ligands competing for the metal, and new experiments will be designed to discriminate between ... |
author2 |
Qualité et fonctionnement hydrologique des systèmes aquatiques (UR QHAN) Centre national du machinisme agricole, du génie rural, des eaux et forêts (CEMAGREF) GEOGIA INSTITUTE OF TECHNOLOGY ATLANTA USA Partenaires IRSTEA Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA) |
format |
Article in Journal/Newspaper |
author |
Tusseau-Vuillemin, M.H. Gilbin, R. Taillefert, M. |
author_facet |
Tusseau-Vuillemin, M.H. Gilbin, R. Taillefert, M. |
author_sort |
Tusseau-Vuillemin, M.H. |
title |
A dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices |
title_short |
A dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices |
title_full |
A dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices |
title_fullStr |
A dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices |
title_full_unstemmed |
A dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices |
title_sort |
dynamic numerical model to characterize labile metal complexes collected with diffusion gradient in thin films devices |
publisher |
HAL CCSD |
publishDate |
2003 |
url |
https://hal.inrae.fr/hal-02581397 https://doi.org/10.1021/es025839o |
genre |
DML |
genre_facet |
DML |
op_source |
ISSN: 0013-936X EISSN: 1520-5851 Environmental Science and Technology https://hal.inrae.fr/hal-02581397 Environmental Science and Technology, American Chemical Society, 2003, 37 (8), pp.1645-1652. ⟨10.1021/es025839o⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.1021/es025839o hal-02581397 https://hal.inrae.fr/hal-02581397 doi:10.1021/es025839o IRSTEA: PUB00011571 |
op_doi |
https://doi.org/10.1021/es025839o |
container_title |
Environmental Science & Technology |
container_volume |
37 |
container_issue |
8 |
container_start_page |
1645 |
op_container_end_page |
1652 |
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1766397541489836032 |