Over the last two decades, there has been widespread international interest in the development of the molten salt reactor concept due to its passive safety, high coolant boiling temperature, low operational pressure, high thermal efficiency, and ease of breeding. Terrestrial Energy Incorporated (TEI) is developing a thermal-spectrum converter type molten salt reactor, called the Integral Molten Salt Reactor (IMSR-400) to be built by 2030. A physics experiment is needed in order to validate the theoretical predictions of the temperature reactivity coefficients of the IMSR-400. This thesis will determine the feasibility of conducting a subcritical experiment, utilizing a Deuterium-Deuterium Fusion Neutron Source (DD). / Thesis / Master of Science (MSc)

Le procédé de traitement du combustible du réacteur à sels fondus (réacteur de génération IV) est un procédé multi-étape dans lequell’extraction des actinides et des lanthanides utilise la technique d’extraction réductrice. Le développement d’un modèle analytique a montré que la mise en contact du sel combustible LiF-ThF4 avec une phase métallique constituée d'un mélange Bi-Li permet l’extraction sélective et quantitative des actinides dans un premier temps, puis l’extraction quantitative des lanthanides dans un second temps. La maitrise de ce procédé nécessite la connaissance des caractéristiques des phases salines impliquées dans le procédé. Les études des propriétés physico-chimiques des sels fluorures fondus ont permis de développer une technique de mesure de la fluoroacidité dans ces milieux via une mesure potentiométrique. Cette technique a permis d’établir un classement de différents mélanges de fluorures fondus en fonction de leur acidité relative. Par ailleurs, une méthode de détermination de la solvatation de solutés dans ces milieux a également été développée par électrochimie afin d’approfondir la connaissance du sel combustible (en particulier solvatation de ThF4 par les ions F-).L'extraction réductrice met également en jeu une phase métallique liquide. Une technique de préparation de cette phase a été développée par électro-réduction de lithium sur une électrode liquide de bismuth en milieu LiCl-LiF. Cette technique permet un bon contrôle de la fraction molaire de lithium introduite dans le bismuth, paramètre essentiel à l’efficacité de l’extraction.Enfin, afin d'optimiser le procédé général de traitement multi-étapes, des méthodes électrochimiques ont été proposées afin de régénérer les différentes phases liquides (salines et métalliques) mise en jeu lors de l’extraction. / The fuel reprocessing of the molten salt reactor (Gen IV concept) is a multi-steps process in which actinides and lanthanides extraction is performed by a reductive extraction technique. The development of an analytic model has showed that the contact between the liquid fuel LiF-ThF4 and a metallic phase constituted of Bi-Li provide firstly a selective and quantitative extraction of actinides and secondly a quantitative extraction of lanthanides. The control of this process implies the knowledge of saline phase properties. Studies of the physico-chemical properties of fluoride salts lead to develop a technique based on potentiometric measurements to evaluate the fluoroacidity of the salts. An acidity scale was established in order to classify the different fluoride salts considered.Another electrochemical method was also developed in order to determine the solvation properties of solutes in fluoride F- environment (and particularly ThF4 by F-)In reductive extraction technique, a metallic phase is also involved. A method to prepare this phase was developed by electro-reduction of lithium on a bismuth liquid cathode in LiCl-LiF melt. This technique allows to accurately control the molar fraction of lithium introduced into the liquid bismuth, which is a main parameter to obtain an efficient extraction.

A breed-and-burn molten salt reactor (BBMSR) concept is proposed to address the Generation IV fuel cycle sustainability objective in a once-through cycle with low enrichment and no reprocessing. The BBMSR uses separate fuel and coolant molten salts, with the fuel contained in assemblies of individual tubes that can be shuffled and reclad periodically to enable high burnup. In this dual-salt configuration, the BBMSR may overcome several limitations of previous breed-and-burn (B$\&$B) designs to achieve high uranium utilisation with a simple, passively safe design. A central challenge in design of the BBMSR fuel is balancing the neutronic requirement of large fuel volume fraction for B$\&$B mode with the thermal-hydraulic requirements for safe and economically competitive reactor operation. Natural convection of liquid fuel within the tubes aids heat transfer to the coolant, and a systematic approach is developed to efficiently model this complex effect. Computational fluid dynamics modelling is performed to characterise the unique physics of the system and produce a new heat transfer correlation, which is used alongside established correlations in a numerical model. A design framework is built around this numerical model to iteratively search for the limiting power density of a given fuel and channel geometry, applying several defined temperature and operational constraints. It is found that the trade-offs between power density, core pressure drop, and pumping power are lessened by directing the flow of coolant downwards through the channel. Fuel configurations that satisfy both neutronic and thermal-hydraulic objectives are identified for natural, 5$\%$ enriched, and 20$\%$ enriched uranium feed fuel. B$\&$B operation is achievable in the natural and 5$\%$ enriched versions, with power densities of 73 W/cm$^3$ and 86 W/cm$^3$, and theoretical uranium utilisations of 300 $\mathrm{MWd/kgU_{NAT}}$ and 25.5 $\mathrm{MWd/kgU_{NAT}}$, respectively. Using 20$\%$ enriched feed fuel relaxes neutronic constraints so a wider range of fuel configurations can be considered, but there is a strong inverse correlation between power density and uranium utilisation. The fuel design study demonstrates the flexibility of the BBMSR concept to operate along a spectrum of modes ranging from high fuel utilisation at moderate power density using natural uranium feed fuel, to high power density and moderate utilisation using 20$\%$ uranium enrichment.