Thermal Conductivity of UO₂ with Defects via DFT+U Calculation and Boltzmann Transport Equation

Accurate evaluation of the thermal conductivity of UO₂ with defects is very significant for optimizing fuel performance and enhancing the safety design of reactors. We employed a method that combines the Boltzmann transport equation with DFT+U to calculate the thermal conductivity of UO₂ containing fission products and irradiation-induced point defects. Our investigation reveals that the thermal conductivity of UO₂ is influenced by defect concentration, defect type, and temperature. Fission products and irradiation defects result in a decrease in thermal conductivity, but they have markedly different impacts on phonon scattering mechanisms. Metal cations tend to scatter low-frequency phonons (less than 5.8 THz), while the fission gas xenon scatters both low-frequency and high-frequency phonons (greater than 5.8 THz), depending on its occupancy at lattice sites. Uranium vacancies scatter low-frequency phonons, while oxygen vacancies scatter high-frequency phonons. When uranium and oxygen vacancies coexist, they scatter phonons across the entire frequency spectrum, which further results in a significant reduction in the thermal conductivity of UO₂. Our calculated results align well with experimental data across a wide temperature range and provide fundamental insights into the heat transfer mechanisms in irradiated UO₂. These findings are essential for establishing a thermal conductivity database for UO₂ under various irradiation conditions and benefit the development of advanced high-performance UO₂ fuel.