High Performance Fuels for Water-Cooled Reactor Systems

Abstract: Investigation of nitride fuels and their properties has, for decades, been propelled on the basis of their desirable high metal densities and high thermal conductivities, both of which oer intrinsic advantages to performance, economy, and safety in fast and light water reactor systems. In this time several key obstacles have been identied as impeding the implementation of these fuels for commercial applications; namely chemical interactions with air and steam, the noted diculty in sintering of the material, and the high costs associated with the enrichment of 15N. The combination of these limitations, historically, led to the well founded conclusion that the most appropriate use of nitride fuels was in the fast reactor fuel cycle, where the cost burdens associated with them is substantially less. Indeed, it is within this context that the vast majority of work on nitrides has been and continues to be done.Nevertheless, following the 2011 Fukushima-Daiichi nuclear accident, a concerted governmental-industrial eort was embarked upon to explore the alternatives of so-called \accident tolerant" and \high performance" fuels. These fuels would, at the same time, improve the response of the fuel-clad system to severe accidents and improve the economy of operation for light water reactor systems. Among the various candidates proposed are uranium nitride, uranium silicide, and a third \uranium nitride-silicide" composite featuring a mixture of the former.In this thesis a method has been established for the synthesis, fabrication, and characterization of high purity uranium nitride, and uranium nitride-silicide composites, prepared by the spark plasma sintering (SPS) technique. A specic result has been to isolate the impact of the processing parameters on the microstructure of representative fuel pellets, essentially permitting any conceivable microstructure of interest to be fabricated. This has enabled the development of a highly reproducible technique for the production of pellets with microstructures tailored towards any desired porosity between 88-99.9%TD, any grain size between 6-24 μm, and, in the case of  the uranium nitride-silicide composite, a silicide-coated UN matrix. This has permitted the evaluation of these microstructural characteristics on the performance of these materials, specically with respect to their role as accident tolerant fuels. This has generated results which have tightly coupled nitride performance with pellet microstructure, with important implications for the use of nitrides in water-cooled reactors.