Abstract
High concentrations of U and 226Ra, and elevated 234U/ 238U activity ratios have been measured in groundwater samples collected from water supply wells and exploratory boreholes in the area surrounding the Underground Research Laboratory (URL) of Atomic Energy of Canada Limited, in southeastern Manitoba. All groundwaters come from the Lac du Bonnet granite batholith or sediments overlying the batholith. Uranium concentrations attain almost 1 mg/l in some shallow, low-salinity groundwaters, whereas 226Ra tends to be high (up to 38 Bq/l) in deeper, saline waters. The U concentrations are some of the highest observed in global groundwaters, yet no significant ore body or mineralization is known in the area. Analyses of unaltered rock samples of the Lac du Bonnet granite show slight U enrichment over average Canadian Shield granites (6.5 μg/g vs 4 μg/g), and altered wall rock in fracture zones is enriched in U by up to an order of magnitude compared to adjacent bedrock. Low 234U/ 238U activity ratios in this altered rock indicate active and recent leaching of U by groundwater. The key control on U concentration appears to be redox potential. Concentrations of U in rock, residence time and groundwater composition are of lesser importance. Geochemical modelling of the shallower, oxidized waters indicates that U speciation consists mainly of anionic carbonate complexes of the uranyl ion. This is supported by the remarkable efficiency of an anionic filter developed to remove high levels of U from drinking water in the area. In more reducing groundwaters, U concentrations are similar to those determined in recent experimental work on uraninite solubility in the pH range 7–8.5. Colloidal U is <10% of total U and organic complexation is unlikely to be significant because of low dissolved organic concentrations. The results emphasize the significance of redox potential in controlling U mobility in both oxidizing and reducing environments and indicate the usefulness of U concentration in estimating groundwater Eh.
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