Aqueous inorganic uranium speciation in European stream waters from the FOREGS dataset using geochemical modelling...

The concentration of the bioavailable uranium fraction (U_bio) at the European scale was deduced by geochemical modelling considering several definitions found in the literature and the FOREGS European stream waters geochemical atlas dataset to produce a U_bio baseline. A sensitivity analysis was performed using three thermodynamic databases. We also investigated the link between total dissolved uranium (U_aq) concentrations, speciation and global stream water chemistry on the one hand, and the lithology and ages of the surrounding rocks on the other. The more U-enriched the stream sediments or rock type contexts are, which tends to be the case with rocks containing silicates (4.1 mg/kg), the less U-concentrated the stream waters are (0.15 μg/L). Sedimentary rocks lead to slightly higher U_aq concentrations (0.34 μg/L) even if the concentration in sediment (U_sed) is relatively low (1.6 mg/kg). This trend is reversed for U_bio, with higher concentrations in a crystalline context. The mean estimated U_bio value ranges from 1.5.10^-3 to 65.3 ng/L and can fluctuate by 3 orders of magnitude depending on the considered definition as opposed to by 2 orders of magnitude accountable to differences between thermodynamic databases. The classification of the water in relation to the two surrounding rock lithologies makes it possible to reduce the mean variability for the U_bio concentrations. Irrespective of the definition of U_bio considered, in 59% of cases the U_bio fraction represents less than 1% of U_aq. Several threshold values relating to U_bio were proposed, assuming knowledge only of the aqueous concentrations of the major elements and U_aq.