French, Jarin Collins2023-08-232023-08-232023-08-22vt_gsexam:38391http://hdl.handle.net/10919/116082Energy needs are projected to continue to increase in the coming decades, and with the drive to use more clean energy to combat climate change, nuclear energy is poised to become an important player in the energy portfolio of the world. Due to the unique nature of nuclear energy, it is always vital to have safe and efficient generation of that energy. In current light water reactors, the most common fuel is uranium dioxide (UO2), an oxide ceramic. There is also ongoing research examining uranium-based based metallic fuels, such as uranium-molybdenum (U-Mo) fuels with low uranium (U) enrichment for research reactors as part of a broader effort to combat nuclear proliferation, and uranium-zirconium-based fuels for Generation IV fast reactors. Each nuclear fuel has weaknesses that need to be addressed for safer and more efficient use. Two major challenges of using UO¬2 are the fission gas (e.g. xenon) release and the decreasing thermal conductivity with increasing burnup. In UMo alloys, the major weakness is the breakaway swelling that occurs at high fission densities. The challenges presented by both fuel types are heavily impacted by microstructure, and several studies have identified that the initial microstructure of the fuel in particular (e.g. initial grain size and grain aspect ratio) plays a large role in determining when and how quickly these processes occur. Thus, knowledge of how such initial microstructures evolve is paramount in having stable and predictable fission gas release and thermal conductivity decrease (in UO2) and fuel swelling (in UMo alloys). Mobility is a critical grain boundary (GB) property that impacts microstructural evolution. Existing literature examines GB mobility for a few specific boundaries but does not (in general) identify the anisotropy relationships that this property has. This work first examined the anisotropy in GB mobility, specifically identifying the anisotropy trend for the low-index rotation axes for tilt GBs in BCC γ U, and fluorite UO2 via molecular dynamics simulation. GB mobility is calculated using the shrinking cylindrical grain method, which uses the capillary effect induced by the GB curvature to drive grain growth. The mobilities are calculated for different rotation axes, misorientation angles, and temperatures in these systems. The results indicated that the density of the atomic plane perpendicular to the (tilt) GB plane (which is also perpendicular to the rotation axis) significantly impacts which GB rotation axis has the fastest boundaries. Specifically, the atomic plane that has a higher density tends to have a faster mobility, because it is more efficient for atoms moving across the GB along such planes. For example, for body-centered cubic materials, the <110> tilt GBs are determined to have the fastest mobilities, while face-centered cubic (FCC) and FCC-like structures such as fluorite have <111> tilt GBs as the fastest. Knowledge of GB mobility and its anisotropy in pure materials is helpful as a baseline, but real materials have solutes or impurities (both intentionally and unintentionally) which are known to affect GB mobility by processes such as solute drag and Zener pinning. Additionally, in reactors, nuclear fission can produce many fission products, each of which acts as an additional impurity that will interact with the GB in some way. Because the initial microstructure and its subsequent evolution are vital for addressing the challenges of using nuclear fuel as described above, knowledge of the impacts of these impurities on GB mobility is required. Therefore, this work examined the impact of solutes and impurities on GB mobility and its anisotropy. In particular, the solute effect was examined using the UMo alloy system, while the impurity effect was examined using Xe (a very common fission product) in the γ U, UMo, and UO2 systems. It is found that both Mo and Xe can cause a solute drag effect on GB mobility in the γ U system, with the effect of Xe being stronger than Mo at the same solute/impurity concentration. Xe also causes a solute drag effect in UO2, though the magnitude of the effect is interatomic-potential-dependent. The mobility anisotropy trend was found to disappear at high solute and impurity concentrations in the metallic U and UMo systems but was largely unaffected in the UO2 system. These results not only increase our fundamental understanding of GB mobility, its anisotropy, and solute/impurity drag effects, but also can be used as inputs for mesoscale simulations to examine polycrystalline grain growth with anisotropic GB mobility and in turn examine how the fuel performance parameters change with these properties.ETDenCreative Commons Attribution 4.0 InternationalGrain boundary mobility anisotropysolute draguranium alloysuranium dioxidemolecular dynamics simulationDissertation