Etude de la migration de l'uranium en milieu naturel : approche expérimentale et modélisation géochimique

Abstract : The present study deals with characterizing uranium migration in a limited zone of Le Bouchet site, a former uranium ore treatment facility, which is dismantled and the rehabilitation of which is under process. Some wastes are packed in a rehabilitated disposal nearby, called the Itteville site. In the framework of the monitoring of the deposit environment (air, water, sediment) set by prefectorial decrees, a piezometer (PZPK) located downstream to the latter, has shown total dissolved uranium peaks each winter since the 1990's. PZPK collects both the interstitial water of a calcareous peat formation, between the surface and 3 m, and an alluvial aquifer near 6 m of depth. Firstly, a hydrogeochemical characterization of the site has evidenced the uranium source term, which is present in the peat soil near 0.8 m, hence excluding any leaching from the waste disposal. Actually, a few microparticles of uranium oxide and mixed uranium-thorium oxide have been detected, but they do not represent the major part of the source term. Secondly, water chemistry of the peat soil water and PZPK has been monitored every two months from 2004 to 2007 in order to understand the reasons of the seasonal fluctuations of [U]tot.diss.. Completed with geochemical modeling and a bacterial identification by 16S rDNA sequence analysis, water chemistry data showed an important sulfate-reducing bacterial activity in summertime, leading to reducing conditions and therefore, a total dissolved uranium content limited by the low solubility of uraninite UIVO2(s). In wintertime, the latter bacterial activity being minimal and the effective pluviometry more important, conditions are more oxidant, which favors U(VI), more soluble, notably as the Ca2UO2(CO3)3(aq) complex, evidenced by TRLFS. Finally, bacterial activity has been reproduced in laboratory in order to better characterize its impact on uranium solubility in the peat soil. Various parameters were tested (C sources, temperature, nutrients) to recreate conditions close and also different to those in situ. 16S rDNA sequence bacterial identifications, throughout the incubation time, have confirmed an increase of sulfate-reducing bacteria proportion. At the same time, water chemistry, as well as geochemical calculations and SEM observations and XANES analyses, have evidenced an decrease of [U]tot.diss., owing to its reduction as UO2(s) (certainly as nanoparticles). Even though the reaction mechanism could not be determined, that is to say biotic (direct uranium reduction by bacteria) or abiotic (indirect reduction), these experiments have showed that sulfate-reducing bacteria can prevail among a varied indigenous population in conditions close to those in situ. Moreover, the studied calcareous peat contains a significant amount of weddellite (CaC2O4.2H2O(s)), accounting for a permanent input of oxalate ions C2O42- which can be used as C source in the course of sulfate and/or uranium reduction in the summer.
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Vannapha Phrommavanh. Etude de la migration de l'uranium en milieu naturel : approche expérimentale et modélisation géochimique. Géochimie. Université Joseph-Fourier - Grenoble I, 2008. Français. ⟨tel-00356619v2⟩

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