Dissolution rate of alpha-doped UO2 in natural groundwater

The objective of this work is to determine whether the presence of trace elements in natural groundwaters affects the dissolution rate of uranium dioxide in the presence of alpha radiation that causes radiolysis of water. The study is a part of the project Reducing Uncertainty in Performance Prediction (REDUPP) under the Seventh Framework Programme of the European Atomic Energy Community (EURATOM). The project aims to reduce uncertainties related to the extrapolation of the results of laboratory experiments to the conditions expected under geologic disposal. Thus far, synthetic groundwater has been normally used in the experiments. The synthetic groundwaters used do not contain all of the chemical elements that occur in natural groundwaters. Three natural groundwaters were chosen for the dissolution experiments with 0%, 5%, and 10% 233U-doped UO2 samples. These include a brackish groundwater, a saline groundwater and a low ionic strength groundwater. At the time of writing this paper, the dissolution experiments have been finished in the first groundwater, which was a moderately saline, brackish groundwater. The groundwater samples for the experiments were taken from a borehole in the Olkiluoto site in Finland. The measurements for dissolution rates were conducted under reducing conditions established using metallic iron in solution and an argon atmosphere in the glove box. The isotope dilution method was used to decrease uncertainties due to precipitation and sorption effects. The resulting dissolution rates in OL-KR6 natural groundwater were generally somewhat higher than the rates measured previously in synthetic groundwaters under similar redox conditions. No clear effect of alpha radiolysis could be seen for tests with lower SA/V, while those for higher SA/V indicated that the dissolution rate was higher for the 10% 233U-doped UO2, suggesting the effect of alpha radiolysis under these conditions.