Abstract

Thorium dioxide is an important material for the nuclear industry. In the last decade, there has been a renewal of interest in studying the feasibility of thorium based fuel reactor to decrease the minor actinides production during the burn-up. Furthermore the resistance of the thorium dioxide to aqueous corrosion can make this material attractive for immobilizing tetravalent actinides. Leaching tests of powdered samples of thorium dioxide calcinated at 1300°C showed that the normalized dissolution rate is very low (between 10−6 and 10−7 g/(m2.d) in acidic media, and 10−9–10−10 g/(m2.d) after pH>3 when the formation of colloïdes occurs. Thorium dioxide which is isomorphic with the actinide dioxides such as UO2, PuO2 allows the formation of solid solutions whatever the concentration of the actinide. Several solid solutions Th1−xUxO2 were synthesized with mole-ratios Th/(U+Th) ranging from x = 0 to 1. X-ray powder diffraction data allowed to check that the Vegard’s law is respected in all the range, and specific surface area was also measured. The resistance of the solid-solution to aqueous corrosion was measured as a function of several parameters (leaching time, leachate acidity, uranium concentration) and the kinetics of solid solutions dissolution was determined as a function of the uranium concentration. The stoechiometry of the release of both actinides was verified, however due to the oxidization of U (IV) in U (VI) in contact with the leachate, the dissolution rate of both thorium and uranium increases with the thorium substitution in the solid by uranium (TV).

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