Testing of Uranium Dioxide Containing Different Levels of Alpha Activity Under Anaerobic and Reducing Conditions

Abstract

AbstractSweden plans to dispose of spent nuclear reactor fuel in a deep geologic repository in granitic rock. The conditions in the repository in the long term will be reducing and water is not expected to contact the fuel until after more than 1000 years. At that time, most of the beta- and gamma-active nuclides will have decayed away and the radiation will be dominated by alpha decay. In order to simulate the radiolysis field for dissolution of spent fuel with age more than 1000 years we have used uranium dioxide containing 5% U-235 and 0, 5, or 10% U-233. The 10% U-233 gives an alpha activity appropriate to about 3000 years after disposal. Samples were testied in a synthetic groundwater with low ionic strength and with the chemical composition dominated by sodium bicarbonate and calcium chloride. Tests were run in triplicate using an atmosphere of nitrogen (1atm), hydrogen (10 bar), hydrogen (10 bar) plus an iron strip in the solution, nitrogen (1 atm) plus an iron strip in the solution, hydrogen (10 bar) plus an iron strip in the solution, hydrogen (10 bar) without the iron strip. Each of these test conditions was run for 2 consecutive periods of at least 21 days. The results showed that the dissolution behavior of the samples was the same for both nitrogen atmosphere and hydrogen atmosphere. The amount of U dissolved under these conditions clearly showed the enhancement of dissolution due to oxidation of the sample surface by radiolysis products. When an iron strip was added to the solution, the amount of dissolution decreased dramatically indicating that the Fe(II) ions released from the corroding iron were able to react with most of the radiolysis products before they could oxidize the uranium dioxide surface.