Simultaneous measurement of labile U(VI) concentration and (234U/238U) activity ratio using a Monophos®-based Diffusive Gradients in thin-films sampler
Background: In a context of environmental monitoring around installations related to the nuclear fuel cycle, the Diffusive Gradient in Thin-films (DGT) technique captures the integrated concentration of U isotopes in their native environment, yielding comprehensive data on U origin (anthropogenic vs...
| Autores: | , , , , , , |
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| Tipo de recurso: | artículo |
| Estado: | Versión publicada |
| Fecha de publicación: | 2024 |
| 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:10459.1/466941 |
| Acceso en línea: | https://doi.org/10.1016/j.aca.2024.343266 https://hdl.handle.net/10459.1/466941 |
| Access Level: | acceso abierto |
| Palabra clave: | Diffusive Gradients in Thin-films (DGT) Field application Inorganic speciation Intercomparison |
| Sumario: | Background: In a context of environmental monitoring around installations related to the nuclear fuel cycle, the Diffusive Gradient in Thin-films (DGT) technique captures the integrated concentration of U isotopes in their native environment, yielding comprehensive data on U origin (anthropogenic vs natural), total concentration, and mobility. However, for common deployment times (4–5 days) in moderately basic waters, none of the commercially available binding gels is adapted to measure the total U concentration. So, the development of novel DGT binding gels is timely. Results: A new DGT sampler, using the Monophos® resin, as well as a new model for the interpretation of the DGT flux, has been successfully developed to measure the labile U concentration (which was also its total concentration) in moderately basic waters (pH ≈ 8). The model accounts for the penetration of uranyl carbonate complexes into the binding gel. Monophos-DGT samplers were able to quantify the total U concentration (accuracy >90 %) in three different mineral basic waters and in a synthetic seawater in laboratory experiments, as well as in situ in the rivers Essonne and Œuf, France. Ion interferences (e.g., Ca2+, Mg2+ and HCO3−), critical when using Chelex and Metsorb resins as binding agents, were overcome by using the new DGT sampler, thus allowing for a longer linear accumulation of U in the tested matrices and, above all, a better detection of U minor isotopes improving the potential of using DGT samplers for water source tracing through isotopic measurements. Significance: The use of the new DGT sampler and the new model for the interpretation of DGT flux is recommended to improve the accuracy of total U concentration determinations in field applications. Moreover, simultaneous elemental and isotopic measurements were successfully performed during field application, confirming new perspectives for environmental applications such as identification of U pollution sources by using isotopic signatures. |
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