Atomistic and cluster dynamics modeling of fission gas (Xe) diffusivity in TRISO fuel kernels

TRISO fuel particles are candidates for use in next generation reactors including gas reactors, fluoride salt-cooled high temperature reactors, and micro-reactors. The UCO fuel kernel consists of a uranium dioxide (UO2) and uranium carbide mixture. The addition of UC2 helps suppress the formation of carbon monoxide gas, which led to failures during initial TRISO development. The addition of uranium carbide alters the chemistry of the UO2 kernel, which is known to influence performance parameters such as fission gas diffusivity, although the impact has not been quantified and no models exist that take the change in chemistry into account. Therefore, better understanding and more accurate models of the impact of chemistry on fuel performance are of high priority. In this paper, a first-principles density functional theory (DFT) and empirical potential based multi-scale study has been carried out to model the diffusivity of fission gas xenon (Xe) in UCO TRISO fuel kernels. The focus is on the UO2 component in the UCO fuel kernels, as that represents the largest volume fraction of the fuel kernels. The study relies on DFT and empirical potential calculations to determine Xe and point defect properties, which are then used in thermodynamic and kinetic models to predict diffusion for intrinsic conditions. In addition, the information is utilized in cluster dynamics simulations using the Centipede code to estimate the impact of irradiation on defect transport. The presence of UC2 or UC2−x in the UCO fuel kernels is shown to have a substantial impact on the UO2 non-stoichiometry by inducing oxygen vacancies and driving UO2 sub-stoichiometric, which causes much slower Xe diffusion in UCO compared to light water reactor UO2 fuel. The application of this model in fuel performance simulations using the Bison code is also demonstrated.