COMPARISON BETWEEN EXPERIMENTALLY MEASURED AND THERMODYNAMICALLY CALCULATED SOLUBILITIES OF UO2AND THO2IN KURT GROUND WATER

2009 
Solubility of a radionuclide is important for defining the release source term of a radioactive waste in the safety and performance assessments of a radioactive waste repository. When the pH and redox potential of the KURT groundwater were changed by an electrical method, the concentrations of uranium and thorium released from UO₂(cr) and ThO₂(cr) at alkali pH (8.1 ~ 11.4) and reducing potential (Eh -7 mole/L. Unexpectedly, the concentration of tetravalent thorium is slightly higher than that of uranium at pH = 8.1 and Eh= -0.2 V conditions, and this difference may be due to the formation of hydroxide-carbonate complex ions. When UO₂(s) and UO₂(am, hyd.), and ThO₂(s) and Th(OH)₄(am) were assumed as solubility limiting solid phases, the concentrations of uranium and thorium in the KURT groundwater calculated by the PHREEQC code were comparable to the experimental results. The dominating aqueous species of uranium and thorium were presumed as UO₂(CO₃)₃ 4- and Th(OH)₃CO₃ - at pH = 8.1 ~ 9.8, and UO₂(OH)₃- and Th(OH)₄(aq) at pH = 11.4.
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