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. / Under artionden har forskning om nitridbranseln och dess egenskaper bedrivits pa grundval av nitridbransletsatravarda egenskaper avseende dess hoga metall tathet och hog varmeledningsformaga. Dessa egenskaper besitter vasentliga fordelar avseende prestanda, ekonomi och sakerhet for metallkylda som lattvatten reaktorer. Genom forskning har aven centrala begr ansningar identierats for implementering av nitridbranslen for kommersiellt bruk. Begransningar avser den kemiska interaktionen med luft och vattenanga, en uppmarksammad svarighet att sintring av materialet samt hoga kostnader forknippade med den nodvandiga anrikningen av 15-N. Kombinationen av dessa begransningar resulterade, tidigare, i en valgrundad slutsats att nitridbranslet mest andamalsenliga anvandningsomrade var i karnbranslecykeln for snabba reaktorer. Detta da kostnaderna forenade med implementeringen av branslet ar avsevart lagre. Inom detta sammanhang har majoriteten av forskning avseende nitrider bedrivits och fortskrider an idag. Dock, efter karnkraftsolyckan i Fukushima-Daiichi 2011, inleddes en samlad industriell och statlig anstrangning for att undersoka alternativ till sa kallade \olyckstoleranta" och \hogpresterande" branslen. Dessa branslen skulle samtidigt forbattra reaktionstiden for bransleinkapsling systemet mot allvarliga olyckor samt forbattra driftsekonomin av lattvattenreaktorer. Foreslagna kandidater ar urannitrid, uransilicid och en tredje \uran nitrid-silicid", komposit bestaende av en blandning av de foregaende. Genom denna avhandling har en metod faststallts for syntes, tillverkning och karaktarisering av uran nitrid av hog renhet samt uran nitrid-silicid kompositer, forberedda med tekniken SPS (Spark Plasma Sintering). Ett specikt resultat har varit att isolera eekten av processparametrar pa mikrostrukturen pa representativa branslekutsar. Detta mojliggor, i princip, framstallningen av alla tankbara mikrostrukturer utav intresse for tillverkning. Vidare har detta mojliggjort utvecklingen av en hogeligen reproducerbar teknik for framstallningen av branslekutsar med mikrostrukturer skraddarsydda for onskad porositet mellan 88 och 99.9 % TD, och kornstorlek mellan 6 och 24 μm. Dartill har en metod for att belagga en matris av uran nitrid-silicid framarbetats. Detta har mojliggjort utvarderingen av dessa mikrostrukturella parametrars paverkan pa materialens prestanda, sarskilt avseende dess roll som olyckstoleranta branslen. Detta har genererat resultat som ar tatt sammanlankat nitridbranslets prestanda till kutsens mikrostruktur, med viktiga konsekvenser for den potentiella anvandningen av nitrider i lattvatten reaktorer. / <p>QC 20170210</p>
| Identifer | oai:union.ndltd.org:UPSALLA1/oai:DiVA.org:kth-201604 |
| Date | January 2016 |
| Creators | Johnson, Kyle D. |
| Publisher | KTH, Reaktorfysik, Stockholm, Sweden |
| Source Sets | DiVA Archive at Upsalla University |
| Language | English |
| Detected Language | English |
| Type | Doctoral thesis, comprehensive summary, info:eu-repo/semantics/doctoralThesis, text |
| Format | application/pdf |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | TRITA-FYS, 0280-316X ; 2016:72, info:eu-repo/grantAgreement/EC/FP7/295825 |
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