To assure nuclear power sustainability, ongoing efforts on advanced closed-fuel cycle options and adapted open cycles have led to investigations of various strategies involving utilization of Transuranic (TRU) nuclides in nuclear reactors. Due to favorable performance characteristics, multiple studies are focused on transmutation options using High Temperature Gas-cooled Reactors (HTGRs). Prismatic HTGRs allow for 3-Dimensional (3D) fuel shuffling and prior shuffling algorithms were based on experimental block movement and/or manual block shuffle patterns. In this dissertation, a physics based 3D multi-directional reloading algorithm for prismatic deep burn very high temperature reactors (DB-VHTRs) was developed and tested to meet DB-VHTR operation constraints utilizing a high fidelity neutronics model developed for this dissertation. The high fidelity automated neutronics model allows design flexibility and metric tracking in spatial and temporal dimensions. Reduction of TRUs in DB-VHTRs utilizing full vectors of TRUs from light water reactor spent nuclear fuel has been demonstrated for both a single and two-fuel composition cores. Performance of the beginning-of-life and end-of-life (EOL) domains for multi-dimensional permutations were evaluated. Utilizing a two-fuel assembly permutation within the two-fuel system domain for a Single-Fuel vector, the developed shuffling algorithm for this dissertation has successfully been tested to meet performance objectives and operation constraints.

The closure of the nuclear fuel cycle is a topic of interest in the sustainability context of nuclear energy. The implication of such closure includes considerations of nuclear waste management. This originates from the fact that a closed fuel cycle requires recycling of useful materials from spent nuclear fuel and discarding of non-usable streams of the spent fuel, which are predominantly the fission products. The fission products represent the near-term concerns associated with final geological repositories for the waste stream. Long-lived fission products also contribute to the long-term concerns associated with such repository. In addition, an ultimately closed nuclear fuel cycle in which all actinides from spent nuclear fuels are incinerated will result in fission products being the only source of radiotoxicity. Hence, it is desired to develop a transmutation strategy that will achieve reduction in the inventory and radiological parameters of significant fission products within a reasonably short time. In this dissertation, a transmutation strategy involving the use of the VHTR is developed. A set of specialized metrics is developed and applied to evaluate performance characteristics. The transmutation strategy considers six major fission products: 90Sr, 93Zr, 99Tc, 129I, 135Cs and 137Cs. In this approach, the unique core features of VHTRs operating in equilibrium fuel cycle mode of 405 effective full power days are used for transmutation of the selected fission products. A 30 year irradiation period with 10 post-irradiation cooling is assumed. The strategy assumes no separation of each nuclide from its corresponding material stream in the VHTR fuel cycle. The optimum locations in the VHTR core cavity leading to maximized transmutation of each selected nuclides are determined. The fission product transmutation scenarios are simulated with MCNP and ORIGEN-S. The results indicate that the developed fission product transmutation strategy offers an excellent potential approach for the reduction of inventories and radiological parameters, particularly for long-lived fission products (93Zr, 99Tc, 129I and 135Cs). It has been determined that the in-core transmutation of relatively short-lived fission products (90Sr and 137Cs) has minimal advantage over a decay-only scenario for these nuclides. It is concluded that the developed strategy is a viable option for the reduction of radiotoxicity contributions of the selected fission products prior to their final disposal in a geological repository. Even in the cases where the transmutation advantage is minimal, it is deemed that the improvement gained, coupled with the virtual storage provided for the fission products during the irradiation period, makes the developed fission product transmutation strategy advantageous in the spent fuel management scenarios. Combined with the in-core incineration options for TRU, the developed transmutation strategy leads to potential achievability of engineering time scales in the comprehensive nuclear waste management.

Des travaux expérimentaux et théoriques ont été menés afin d’enrichir la connaissance et la compréhension du comportement en corrosion du carbure de silicium en présence de mélanges gazeux complexes à très hautes températures. A cette fin ont été mis au point deux nouvelles méthodes expérimentales basées sur le chauffage par effet Joule pour le suivi in-situ des cinétiques d’oxydation, ainsi qu’un modèle intégrant thermodynamique hétérogène et phénomènes de transport en phase gazeuse. Dans le domaine des hautes températures et des basses pressions partielles en espèces oxydantes, l’oxydation de SiC est dite « active » et se traduit par la formation de produits gazeux et la dégradation rapide du matériau associée à une cinétique limitée par le transport des espèces en phase gazeuse. Dans le domaine des basses températures et des hautes pressions partielles en espèces oxydantes, l’oxydation est dite « passive » et se traduit par la croissance d’une couche d’oxyde condensé SiO2 qui agit comme une barrière de diffusion vis-à-vis des espèces oxydantes, et dont la croissance fait intervenir une variété de phénomènes physico-chimiques qu’il a été nécessaire de découpler.Une attention particulière a été portée à l’étude de la transition entre les domaines de conditions correspondant à chacun de ces modes d’oxydation dans des mélanges simples et dans des mélanges complexes comportant deux espèces oxydantes différentes. Une analyse précise de plusieurs modèles de description théorique de cette transition active/passive a pu être réalisée en s’appuyant sur les nouveaux moyens numériques ainsi que sur les nouveaux éclairages relatifs aux mécanismes d’oxydation active et passive issus de cette étude et de la littérature. / Experimental and theoretical studies have been carried out in order to obtain further knowledge and understanding of the corrosion behavior of silicon carbide under complex gas mixtures at very high temperatures. To that purpose, two original experimental methods based on Joule-heating have been designed for the in-situ following of SiC oxidation kinetics, and a model accounting for both heterogeneous kinetics and gas-phase transport phenomena has been developed thanks to a finite volume method. At high temperatures and low oxidant partial pressure, oxidation of SiC is « active » and associated with the formation of gaseous products and high degradation rates of the original materials, the reaction being rate-determined by species transport through a gaseous boundary layer. At low temperatures and high oxidant partial pressures, oxidation is « passive » and associated with the growth of a condensed oxide scale acting as a protecting diffusion barrier. An analytical study has been conducted in order to try and isolate the effects of the various physical and chemical phenomena involved during this passive oxidation, such as different growth mechanisms, volatilization or bubble formation, and quantify how temperature and gas composition influence them.An experimental study of the active/passive transition in the oxidation of SiC has been conducted under gas mixtures including one or two different oxidant species. Numerical simulation tools as well as new insights on oxidation mechanisms were used to analyze different predictive models of the active/passive transition and evaluate and understand the differences between these theoretical results and the ones obtained experimentally.