Solution composition and particle size effects on the dissolution and solubility of a ThO2 microstructural analogue for UO2 matrix of nuclear fuel

The objective of this study was to investigate the dissolution rate of ThO2 which was synthesised to approximate, as closely as possible, the microstructure of UO2 in a nuclear fuel matrix. The optimal sintering temperature for ThO2 pellets was found to be 1750 ℃, which produced pellets with a microstructure similar to UO2 nuclear fuel pellets, with randomly oriented grains ranging in size from 10 to 30 μm. Dissolution was conducted using ThO2 particles of different size fractions (80 to 160 μm and 2 to 4 mm) in the presence and absence of carbonate, in solutions with pH from 2 to 8 and at 80 ℃. Dissolution rates were calculated from Th released from the solid phase to solution. Particles of ThO2 were also leached with 1 M HNO3 at 80 ℃ in order to investigate the morphological changes at the particle surfaces. The concentration of Th was found to be ≥ 10–9 mol/L at pH ≤ 4, lower than the theoretical solubility of crystalline ThO2. At higher pH values, from 4 to 8, the measured concentrations (10−10 to 10–12 mol/L) were between the theoretical solubility of ThO2 and Th(OH)4. Grain boundaries were shown to exert an influence on the dissolution of ThO2 particles. Using high resolution aqueous solution analysis, these data presented here extend the current understanding of Th solubility in solution