The research conducted was a feasibility study using Lithium Fluoride-Beryllium Fluoride (LiF-BeF2) or FLiBe as a coolant with a natural uranium neutron spallation source applied to an accelerator driven sub-critical molten salt reactor. The study utilized two different software tools, MCNPX 2.6 and FLUENT 12.1. MCNPX was used to determine the neutronics and heat deposited in the spallation target structure while FLUENT was used to determine the feasibility of cooling the target structure with FLiBe. Several target structures were analyzed using a variety of plates and large cylinders of natural uranium with a proton beam incident on a Hastelloy-N window. The supporting structures were created from Hastelloy-N due to their anti-corrosive properties of molten salts such as FLiBe and their resistance to neutron damage. The final design chosen was a "Sandwich" design utilizing a section of thick plates followed by several smaller plates then finally a section of thick plates to stop any protons from irradiating the bottom of the target support structure or the containment vessel of the reactor. Utilizing a proton beam with 0.81 MW of proton beam power at 1.35 mA with proton kinetic energies of 600 MeV, the total heat generated in the spallation target was about 0.9 MW due to fissions in the natural uranium. Additionally, the neutrons produced from the final design of the spallation target were approximately 1.25x1018 neutrons per second which were mainly fast neutrons. The use of a natural uranium target proved to be very promising. However, cooling the target using FLiBe would require further optimization or investigation into alternate coolants. Specifically, the final design developed using FLiBe as a coolant was not practically feasible due to the hydraulic forces resulting from the high flow rates necessary to keep the natural uranium target structures cooled. The primary reason for the lack of a feasible solution was the FLiBe as a coolant; FLiBe is unable to pull enough heat generated in the target out of the target structure. Due to the high energy density of a natural uranium spallation target structure, a more effective method of cooling will be required to avoid high hydraulic forces, such as a liquid metal coolant like lead-bismuth eutectic. / Master of Science

This work 1) draws insights on molten salt structure and properties directly from ab initio molecular dynamics (AIMD) simulations, 2) demonstrates the advantageous symbiosis of computational and experimental collaborations on molten salt research, and 3) simultaneously generates ab initio data sets for fitting an interatomic potential model for classical molecular dynamics (MD) simulations. This work discusses the motivations for AIMD simulations of molten salts, thermophysical properties and structural characteristics of interest, advanced methodologies for AIMD simulations, and several completed AIMD studies on molten salts. Of import are the methodological contributions of this work to AIMD simulations, primarily the radical increase in generalized gradient planewave energy cutoff used to more accurately model the electron distribution across a highly-polarizable molten salt. Cutoffs of up to 2500 Rydbergs are used in this work, but 2000 Rydbergs is found to be sufficient for most AIMD NpT modelling of molten fluorides. The equilibrium liquid density of eutectic FLiNaK as a function of temperature is found to agree with the experimental density reported by Chrenkova et al. to within 0.2%, and the equilibrium liquid density of eutectic FMgNaK is found to agree with experimental measurements reported herein to within 4%. Self-diffusion coefficients in FMgNaK are also considered, with applicability to other halide salts. Molybdenum, Cesium, iodide, nickel, hydrogen, oxide, and uranium complexation are examined. It is found that solvation strength can be qualitatively determine via AIMD simulations, and that poorly solvated solutes will minimize the surface area of interaction with the salt solution. Cesium in particular is shown to be volatile or retainable in FLiBe at 500, 650, and 800 ËšC based on complexation and validated experimentally. It is shown that the chemical potential of an anion varies between melts as influenced by the different cations present in each melt. Hence, attempts to use a common electrochemical reference reaction for different salt mixtures are at best an approximation.

This work demonstrates how ICP-MS can be employed to evaluate cesium volatilization from LiF-BeF2 (Flibe) salt with ab initio molecular dynamics studies used as corroborating data to better understand cesium behavior. Using mixtures of Flibe with 2 mol% CsF, it was found that cesium was stable within the salt melt at temperatures between 500-650°C over a time span of 8 hours. At 800°C, cesium vaporized from the salt at a rate of 0.83% / hr with a mass flux of 0.0023 g Cs / cm2hr. The atomistic modeling results show poor solvation of Cs at 500°C and 800°C, with stability preferred at 650°C. Specialized equipment and procedures were needed to enable this work, especially those required for safe handling of beryllium containing salts. The methods, custom equipment, and important considerations for working with high-temperature fluoride salts are detailed in this thesis.

This work primarily centers on measuring the physical properties of molten salts. It's dedicated to outlining the methodology, enhancing measurement methods, and scrutinizing data to uncover insights regarding the interaction between molten salt and solid structures in the context of designing and generating electrical energy in molten salt reactors. The initial phase of this research involved collaborating with Brigham Young University's molecular dynamics simulation group to create an Archimedean density measurement device. This endeavor was primarily geared towards generating empirical data for the purpose of enhancing molecular dynamics simulation data. The tasks encompassed designing and validating the experimental setup, with a particular focus on measuring the densities of a novel salt composition--FMgNaK, a prospective nuclear fuel salt fuel/coolant. In the next chapter, we delve into the development, validation, and significant improvement of the rotational Couette viscosity measurement method at high temperatures. Originally designed for room temperature conditions, the methodology failed to account for the substantial temperature difference between the calibration fluids and the molten salts. Consequently, we introduce a theory aimed at correcting errors stemming from the thermal expansion of the solid container material during the transition from calibration to high temperature fluid measurement. As part of this comprehensive discussion, we also present the correction applied during the validation testing of the viscosity setup, with a specific focus on a nitrate salt known as solar salt. The final experiment development centered on the creation and validation of the Axisymmetric Drop-Shape Analysis (ADSA) method for use with molten salt. However, working with a specific nitrate salt, known as solar salt, posed challenges due to its propensity to wet all common high temperature substrates. This high degree of wetting posed hindrances to several physical properties measurements. Therefore, the primary objective of this work was to identify a non-wetting substrate to enhance the accuracy of ADSA and other measurement methods. Within this context, we present the results of surface tension and contact angle measurements, which were derived from the ADSA method, and the development of a non-wetting substrate for use with solar salt. In the final stage of this research, the ADSA method was applied to FLiBe, a critical fluoride salt in molten salt nuclear reactor design, and tellurium-bearing FLiBe to examine its interaction with boron nitride, a key solid porous material used in reactor vessel structures. Surface tension and contact angle measurements were conducted on various substrates, revealing the influence of oxygen on boron nitride wetting. Additionally, the study confirmed that tellurium, despite its chemical similarity to oxygen, did not significantly affect surface tension or contact angle, ruling out a substantial impact on boron nitride infiltration. The chapter also presents comprehensive data on the surface tension and densities of FLiBe, FLiNaK, and the chloride salt NaCl-KCl.