Fission products in nuclear fuel pellets can affect fuel performance as they change the fuel chemistry and structure. The behavior of the fission products and their release mechanisms are important to the operation of a power reactor. Research has shown that fission product release can occur through grain boundary (GB) at low burnups. Early fission gas release models, which assumed spherical grains with no effect of GB diffusion, did not capture the early stage of the release behavior well. In order to understand the phenomenon at low burnup and how it leads to the later release mechanism, a microstructurally explicit model is needed. This dissertation conducted finite element simulations of the transport behavior using 3-D microstructurally explicit models. It looks into the effects of GB character, with emphases on conditions that can lead to enhanced effective diffusion. Moreover, the relationship between temperature and fission product transport is coupled to reflect the high temperature environment.

The modeling work began with 3-D microstructure reconstruction for three uranium oxide samples with different oxygen stoichiometry: UO2.00 UO2.06 and UO2.14. The 3-D models were created based on the real microstructure of depleted UO2 samples characterized by Electron Backscattering Diffraction (EBSD) combined with serial sectioning. Mathematical equations on fission gas diffusion and heat conduction were studied and derived to simulate the fission gas transport under GB effect. Verification models showed that 2-D elements can be used to model GBs to reduce the number of elements. The effect of each variable, including fuel stoichiometry, temperature, GB diffusion, triple junction diffusion and GB thermal resistance, is verified, and they are coupled in multi-physics simulations to study the transport of fission gas at different radial location of a fuel pellet. It was demonstrated that the microstructural model can be used to incorporate the effect of different physics to study fission gas transport. The results suggested that the GB effect is the most significant at the edge of fuel pellet where the temperature is the lowest. In the high temperature region, the increase in bulk diffusivity due to excess oxygen diminished the effect of GB diffusion.

ABSTRACT The behavior of the fission products, as they are released from fission events during nuclear reaction, plays an important role in nuclear fuel performance. Fission product release can occur through grain boundary (GB) at low burnups; therefore, this study simulates the mass transport of fission gases in a 2-D GB network to look into the effects of GB characteristics on this phenomenon, with emphasis on conditions that can lead to percolation. A finite element model was created based on the microstructure of a depleted UO2 sample characterized by Electron Backscattering Diffraction (EBSD). The GBs were categorized into high (D2), low (D1) and bulk diffusivity (Dbulk) based on their misorientation angles and Coincident Site Lattice (CSL) types. The simulation was run using different diffusivity ratios (D2/Dbulk) ranging from 1 to 10^8. The model was set up in three ways: constant temperature case, temperature gradient effects and window methods that mimic the environments in a Light Water Reactor (LWR). In general, the formation of percolation paths was observed at a ratio higher than 10^4 in the measured GB network, which had a 68% fraction of high diffusivity GBs. The presence of temperature gradient created an uneven concentration distribution and decreased the overall mass flux. Finally, radial temperature and fission gas concentration profiles were obtained for a fuel pellet in operation using an approximate 1-D model. The 100 µm long microstructurally explicit model was used to simulate, to the scale of a real UO2 pellet, the mass transport at different radial positions, with boundary conditions obtained from the profiles. Stronger percolation effects were observed at the intermediate and periphery position of the pellet. The results also showed that highest mass flux happens at the edge of a pellet at steady state to accommodate for the sharp concentration drop.