Concentration of uranium and plutonium in unsaturated spent fuel tests.

Commercial spent fuel is being tested under oxidizing conditions at 90 C in drip tests with simulated groundwater to evaluate its long-term performance in a potential repository at Yucca Mountain [1-4]. The tests allow us to monitor the dissolution behavior of the spent fuel matrix and the release rates of individual radionuclides. This paper reports the U and Pu concentrations in the leachates of drip tests during 3.7 years of reaction. Changes in these concentrations are correlated with changes in the measured pH and the appearance of alteration products on the fuel surface. Although there is little thermodynamic information at 90 C for either uranyl or plutonium compounds, some data are available at 25 C [5-8]. The literature data for the U and Pu solubilities of U and Pu compounds were compared to the U and Pu concentrations in the leachates. We also compare Wilson's [9] U and Pu concentrations in semi-static tests at 85 C on spent fuel with our results