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CC BY V4.0, Open Access
Dissertation
Recovery of Uranium and Thermochemical Analysis of Prospective MSR Materials in Molten Chloride Salts
Washington State University
Doctor of Philosophy (PhD), Washington State University
2023
DOI:
https://doi.org/10.7273/000006376
Abstract
In January 2022, TerraPower and Southern Company agreed to design, construct, and operate the world’s first molten chloride fast reactor at Idaho National Laboratory (INL) by 2025 as part of a rekindling interest in high temperature nuclear reactor technology within the United States. In this work, two thrusts were investigated in the interest of contributing to knowledge that would be valuable to the design of these kinds of reactors: the recovery of additional uranium from spent nuclear fuel after electrorefining and the thermochemistry of molten salts that are of interest for usage as fuel carriers and coolants. Electrochemical deposition with redox replacement (EDRR) of lanthanum with uranium was demonstrated as a complementary technique to electrolysis after electrorefining, showing the selective recovery of dilute concentrations of uranium in molten LiCl-KCl-LaCl3(1wt%)-UCl4(0.15wt%) onto an inert tungsten working electrode. In addition to EDRR, pulse reverse-pulse (PRP) deposition of dilute uranium onto a tungsten working electrode was monitored intermittently with electrochemical impedance spectroscopy (EIS) in the same salt composition. Impedance measurements from EIS were then fitted to an equivalent circuit (EC) model of the physical phenomena occurring at the electrode surface with Simplex optimization to characterize double layer capacitance, charge transfer resistance, Warburg diffusion, and CPE-restricted diffusion of uranium deposits over 600 PRP cycles. Lastly, melting point, heat capacity (Cp), and enthalpy (ΔH & ΔH_fusion) measurements of MgCl2-NaCl were taken between 400 - 800°C using high temperature drop calorimetry and differential scanning calorimetry to contribute to knowledge of the thermophysical properties of chloride salts proposed for use in molten salt reactors.
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Details
- Title
- Recovery of Uranium and Thermochemical Analysis of Prospective MSR Materials in Molten Chloride Salts
- Creators
- Jeffrey Allen Eakin
- Contributors
- Haluk Beyenal (Advisor)Cornelius F Ivory (Committee Member)Xiaofeng Guo (Committee Member)Steven R. Saunders (Committee Member)
- Awarding Institution
- Washington State University
- Academic Unit
- School of Chemical Engineering and Bioengineering
- Theses and Dissertations
- Doctor of Philosophy (PhD), Washington State University
- Publisher
- Washington State University
- Number of pages
- 190
- Identifiers
- 99901087515101842
- Language
- English
- Resource Type
- Dissertation