Water-rock interactions of uranium deposits: A field investigation and laboratory batch experiment

Abstract

Interactions between bedrock and groundwater in the far-field of a deep geological repository (DGR) for high-level radioactive waste significantly affect the transport of uranium, which is the major radionuclide in a DGR. Therefore, the present study evaluated the geochemical behavior of uranium by assessing the hydrogeochemical characteristics of groundwater, surface water, mine water, and quarry runoff water in the Okcheon metamorphic belt, which represents a natural analogue study site in Korea. A batch experiment was also conducted to further elucidate the interactions between the uranium-containing rock and groundwater in the study area. The results of the field investigation indicated that uranium in groundwater formed aqueous complexes in the form of calcium uranyl tricarbonate. The concentrations of uranium in groundwater were low, at less than 1 μg L−1, which seems to be attributable to the dissolutions of uraninite, coffinite, UO2(am), and U4O9(c) under the moderately reduced condition and subsequent control by co-precipitation with iron (hydr)oxides. The results of the batch experiment showed that uranium concentrations may be controlled by adsorption or surface complexation with iron oxides. The field study demonstrates the equilibrium state maintained in the current geochemical conditions at the study site, while the batch experiment provides implications regarding the reaction processes over time. Overall, this study showed that uranium forms complexes with carbonate and sulfate under the geochemical conditions of the study site, and that its mobility could be restricted through co-precipitation or adsorption/surface complexation. This study is expected to contribute to a comprehensive understanding of how the behavior of uranium is affected by the evolution of geochemical conditions around the DGR.