Temporal uranium records of oak tree rings (QuercusPetraea) by(LA)-HR-ICP-MS from a former uranium mining site (Rophin,France)

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U(VI) retention in compact Callovo-Oxfordian clay stone at temperature (20–80 °C); What is the applicability of adsorption models?

International audienceIn the context of the radioactive waste management in deep geological formations, U(VI) retention by intact Callovo-Oxfordian claystone (COx) was studied by percolation-type experiments at 20 and 80 degrees C. The experimental results were confronted with modelling prediction based on a published adsorption model developed from dispersed media in the 20-80 degrees C temperature range. For the experiments at 20 degrees C, the adsorption model allowed to explain the results for the intact system; the retention was weak (R-d similar to 10 L.kg(-1)) and the analysis of the COx phases at the end of the experiment confirmed a retention of U by the clay fraction. The adsorption model in temperature also explained the observed trend of increasing retention with increasing temperature. However, it underestimated the temperature effect on the adsorption of U(VI) by the COx clay fraction, and other phases contributed to the retention. Solid-state analysis of the percolation-doped samples indicated a reactivity in the order pyrite>clay>calcite phases. The transposition of the knowledge at 20 degrees C from the dispersed system to the intact medium was therefore not possible at 80 degrees C for the studied U(VI)/COx system

Temporal uranium records of oak tree rings (QuercusPetraea) by(LA)-HR-ICP-MS from a former uranium mining site (Rophin,France)

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Uranium quantification of oak tree rings (Quercus petraea) from a former uranium mining site by High Resolution Inductively Coupled Plasma Mass spectrometry in Laser Ablation and Solution modes

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Investigation of europium retention on Callovo-Oxfordian clay rock (France) by laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) and percolation experiments in microcells

International audienceClay-rock formations are under investigation in several countries as a potential host of radioactive waste repositories. In order to assess the long-term safety of these concepts, retention distribution data (Rd) are needed to describe the interaction between radionuclides and natural rock. While Rd values obtained from batch-type experiments with dispersed material are essential for the development of retention models, it is also important to generate retention data under more realistic conditions, in particular with compact samples. Specifically, the literature data on strongly retained radionuclides proves to be very scarce. The present study focuses on the retention of europium (Eu) at trace concentrations on clay samples extracted from the Callovo-Oxfordian (COx) formation in France. Rd values obtained with compact COx samples are assessed by a methodology coupling percolation experiments (in pressurized microcells), performed using submillimeter-sized samples in thickness, and Laser Ablation Inductively Coupled Plasma Mass Spectrometry measurements. The Rd found at trace concentrations under non-transient conditions are high (Rd > 104 mL g−1) and in agreement with those recorded under classical batch-type conditions or those deduced from the distribution of naturally-occurring Eu between the pore water and the clay rock. They can be described by modeling with existing sorption databases, considering an adsorption process only on the clay fraction. This was validated by solid state LA-ICP-MS analyses of one of the Eu-spiked COx samples; the added europium was found exclusively in the COx clay fraction

Uranium retention in a Callovo-Oxfordian clay rock formation: From laboratory-based models to in natura conditions

International audienceFor the performance assessment of radioactive waste disposal, it is critical to predict the mobility of radionuclides in the geological barrier that hosts it. A key challenge consists of assessing the transferability of current knowledge on the retention properties deduced from model systems to in natura situations. The case of the redox-sensitive element uranium in the Callovo-Oxfordian clay formation (COx) is presented herein. Extensive experimental work was carried out with respect to parameters affecting uranium speciation (pH, PCO2, [Ca] and redox potential) with illite, COx clay fraction and raw COx claystone. The “bottom-up” approach implemented, with illite and montmorillonite as reactive phases, quantitatively explains the adsorption results of U(VI) and U(IV) on COx. While retention is high for U(IV) (Rd∼104 L kg−1), it remains very low for U(VI) (Rd∼4 L kg−1) due to the formation of soluble ternary Ca(Mg)–U(VI)-carbonate complexes. The applicability of the sorption model was then assessed by comparing predictive analyses with data characterizing the behavior of naturally-occurring U ( 70 L kg−1. (Elsevier

URANIUM BEHAVIOR IN CALLOVO-OXFORDIAN CLAY ROCK FORMATION; FROM LABORATORY-DERIVED MODELS TO IN-SITU KD VALUES

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An integrated approach combining soil profile, records and tree ring analysis to identify the origin of environmental contamination in a former uranium mine (Rophin, France)

International audienceUranium mining and milling activities, raise environmental concerns due to the release of radioactive and other toxic elements. Their long-term management thus requires a knowledge of past events coupled with a good understanding of the geochemical mechanisms regulating the mobility of residual radionuclides. This article presents the results on the traces of anthropic activity linked to previous uranium (U) mining activities in the vicinity of the Rophin tailings storage site (Puy de Dôme, France). An interdisciplinary approach was developed based on a study of the site's history and records, as well as on a radiological and chemical characterization of soil cores and a dendrochronology. Gamma survey measurements of the wetland downstream of the Rophin site revealed a level of 1,050 nSv.h-1. Soil cores extracted in the wetland showed U concentrations of up to 1,855 mg.kg-1, which appears to be associated with the presence of a whitish silt loam (WSL) soil layer located below an organic topsoil layer. Records, corroborated by prior aerial photographs and analyses of 137Cs and 14C activities, suggest the discharge of U mineral particles while the site was being operated. Moreover, lead isotope ratios indicate that contamination in the WSL layer can be discriminated by a larger contribution of radiogeni