Dissolution of UO₂ at various parametric conditions::A comparison between calculated and experimental results

The solubilities of uranium measured in deionized water, in sodium bicarbonate solutions as a function of carbonate concentration and in two types of synthetic groundwaters have been compared with those predicted using the reaction pathway program, PHREEQE. All the measurements were carried out under both air-saturated, oxidizing and anoxic, reducing conditions.The experimental solubility values of uranium under oxidizing conditions are, in general, lower when compared to the corresponding theoretical ones calculated by PHREEQE. A critical factor is the choice of solubility constant for the solid phase. The reason for the lower solubility values may also be the mechanism of dissolution leading for example either to a situation where low dissolution rate is a limiting factor, or to formation of some solid phase of uranium with lower solubility. The experimental solubility values under reducing conditions appear to be in good agreement with the theoretical solubility values