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...
| Autores: | ; ; ; ; ; ; |
|---|---|
| Tipo de documento: | Artículo |
| Estado: | Accepted version |
| 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 |
| Nivel de acceso: | Acceso abierto |
| Palabra clave: | Lability degree Diffusion coefficients Mixture effects |
| _version_ | 1878735122110349313 |
|---|---|
| author | Altier Infantes, Alexandra |
| 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 |
| author_browse | Altier Infantes, Alexandra Cecilia Averós, Joan Galceran i Nogués, Josep Jiménez-Piedrahita, Martín Puy Llorens, Jaume Rey-Castro, Carlos Uribe Kaffure, Ramiro |
| 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 |
| collection | Recercat. Dipósit de la Recerca de Catalunya |
| 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. |
| eu_rights_str_mv | openAccess |
| format | article |
| id | ES_7667a38bddf4f6d12e28dc2a64518c4e |
| institution | 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) |
| network_acronym_str | ES |
| network_name_str | España |
| oai_identifier_str | oai:recercat.cat:10459.1/64774 |
| publishDate | 2018 |
| publishDateSort | 2018 |
| publisher | CSIRO Publishing |
| publisherStr | CSIRO Publishing |
| reponame_str | Recercat. Dipósit de la Recerca de Catalunya |
| spelling | Effects of a mixture of ligands on metal accumulation in diffusive gradients in thin films (DGT) Altier Infantes, Alexandra Jiménez-Piedrahita, Martín Uribe Kaffure, Ramiro Rey-Castro, Carlos Cecilia Averós, Joan Galceran i Nogués, Josep Puy Llorens, Jaume Lability degree Diffusion coefficients Mixture effects 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. 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 Publishing https://doi.org/10.1071/EN17232 http://hdl.handle.net/10459.1/64774 |
| 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 |
| status_str | acceptedVersion |
| title | 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_short | 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) |
| topic | Lability degree Diffusion coefficients Mixture effects |
| topic_facet | Lability degree Diffusion coefficients Mixture effects |
| url | https://doi.org/10.1071/EN17232 http://hdl.handle.net/10459.1/64774 |