Thermal diffusivity and conductivity of thorium- uranium mixed oxides

Abstract

Thorium-uranium oxide pellets with high densities were prepared at the Canadian Nuclear Laboratories (CNL) by co-milling, pressing, and sintering at 2023 K, with UO2 mass contents of 0, 1.5, 3, 8, 13, 30, 60 and 100%. At the Joint Research Centre, Karlsruhe (JRC-Karlsruhe), thorium-uranium oxide pellets were prepared using the spark plasma sintering (SPS) technique with 79 and 93 wt. % UO2. The thermal diffusivity of (Th1-xUx)O2 (0 ≤ x ≤ 1) was measured at CNL and at JRC-Karlsruhe using the laser flash technique. ThO2 and (Th,U)O2 with 1.5, 3, 8 and 13 wt. % UO2 were found to be semi-transparent to the infrared wavelength of the laser and were coated with graphite for the thermal diffusivity measurements. This semi-transparency decreased with the addition of UO2 and was lost at about 30 wt. % of UO2 in ThO2. The thermal conductivity was deduced using the measured density and literature data for the specific heat capacity. The thermal conductivity for ThO2 is significantly higher than for UO2. The thermal conductivity of (Th,U)O2 decreases rapidly with increasing UO2 content, and for UO2 contents of 60% and higher, the conductivity of the thorium-uranium oxide fuel is close to UO2. As the mass difference between the Th and U atoms is small, the thermal conductivity decrease is attributed to the phonon scattering enhanced by lattice strain due to the introduction of uranium in ThO2 lattice. The new results were compared to the data available in the literature and were evaluated using the classical phonon transport model for oxide systems.