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A Radioactive Tracer Dilution Method for Mass Determination in Licl-Kcl Radioactive Eutectic Salts

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A Radioactive Tracer Dilution Method for Mass Determination in Licl-Kcl Radioactive Eutectic Salts A Radioactive Tracer Dilution Method for Mass Determination in LiCl-KCl Radioactive Eutectic Salts THESIS Presented in Partial Fulfillment of the Requirements for the Degree of Masters of Science from the Graduate School of The Ohio State University By Douglas Ernest Hardtmayer, B.Sc. Welding Engineering Graduate Program in Nuclear Engineering The Ohio State University 2018 Thesis Committee: Dr. Lei. Cao, Advisor Dr. Vaibhav Sinha Copyright By Douglas Ernest Hardtmayer 2018 ABSTRACT Radioactive Tracer Dilution (RTD) is a new method where a radioactive tracer isotope is dissolved in a given substance, and the dilution thereof corresponds to the mass and volume of the substance in which the tracer was dissolved. This method is being considered commercially as a means of measuring the mass of Lithium Chloride-Potassium Chloride (LiCl-KCl) eutectic salt in electrorefiners where spent nuclear fuel has been reprocessed. Efforts have been ongoing to find an effective and efficient way of measuring the mass of this salt inside of an electrorefiner for nuclear material accountancy purposes. Various methods, including creating volume calibration curves with water and molten salt, have been tried but have numerous shortcomings, such as needing to recalibrate the fitted volume curve for a specific electrorefiner every time a new piece of equipment is added or removed from the device. Research at The Ohio State University has shown promise using Na22 as a tracer in LiCl-KCl eutectic salt, and that the interference from a common fission product found in an electrorefiners salt, Eu154, could be accounted for, and an accurate mass measurement could be determined. To more closely mimic the conditions in which this technique would be used, Cs137 was added to a larger mass of LiCl-KCl salt, to see if this would affect the measurement of the salt mass. Self-shielding effects were noticed with larger salt masses, and MCNP was utilized to validate and quantify this self-shielding effect. To further Increase this interference, button sources of Cs137 were utilized to artificially raise the Cs137 activity to increase the dead time of a standard High Purity Germanium Detector. It was found that the addition of Cs137, and using a larger salt mass, did not affect the overall methodology used to determine salt mass, and in fact, simulation packages such as MCNP can be further used to increase the accuracy of this methodology. It was also found that idealistic correctional models could account for higher dead times incurred by the introduction of additional Cs137. ii Dedication This document is dedicated to my family and supportive group of many friends. iii Acknowledgements I would like to first thank Dr. Lei (Raymond) Cao, my graduate advisor in the Ohio State Nuclear Engineering program. He has been a tremendous source of inspiration, and was instrumental in supporting me during my time studying at The Ohio State University. I would also like to thank the Ohio State University Research Reactor lab staff, whose hard work and attention detail, provided the data and results that made this study a success. Lastly, I would like to thank our sponsors at the Idaho National Laboratory, who helped to fund and provide insight on this project. iv Vita May 2012……………………………………………Hudson High School, Hudson, OH. Dec. 2016…………………………………………...B.Sc., Welding Engineering, The Ohio State University, Columbus, OH. Jan 2012 to Present…………………………........ Graduate Research Associate, Nuclear Engineering Program, The Ohio State University, Columbus, OH. Publications Lei Cao*, Josh Jarrell**, Andrew Kauffman, Susan White, Kevin Herminghuysen, Douglas Hardtmayer**, Jeff Sanders, Shelly Li. (2017). A Radioactive Tracer Dilution Method to Determine the Mass of Molten Salt. Journal of Radioanalytical and Nuclear Chemistry. doi: 10.1007/s10967-017-5417-5 [Published] Fields of Study Major Field: Nuclear Engineering v Table of Contents ABSTRACT ...................................................................................................................................................... ii Dedication .................................................................................................................................................... iii Acknowledgements ...................................................................................................................................... iv Vita ................................................................................................................................................................ v List of Figures .............................................................................................................................................. vii List of Tables .............................................................................................................................................. viii Introduction .................................................................................................................................................. 1 Theory ........................................................................................................................................................... 5 Radioactive Tracer Dilution ....................................................................................................................... 5 Tracer Selection ........................................................................................................................................ 6 Isotopic Ratio Determination .................................................................................................................... 7 Experimental Procedure ............................................................................................................................... 9 Radioactive Tracer Dilution ....................................................................................................................... 9 Dead Time Measurement ....................................................................................................................... 12 Sensitivity Analysis .................................................................................................................................. 14 Results and Discussion ................................................................................................................................ 15 Radioactive Tracer Dilution Results ........................................................................................................ 15 Preliminary Results ............................................................................................................................. 15 Self-Attenuation Validation ................................................................................................................ 21 Dead Time Measurement and Correction .............................................................................................. 25 Sensitivity study ...................................................................................................................................... 28 Summary ..................................................................................................................................................... 31 Conclusions ............................................................................................................................................. 31 Future Work ............................................................................................................................................ 32 References .................................................................................................................................................. 33 Appendix: Supplemental Information ........................................................................................................ 36 1. MATLAB script for Dead Time Corrections ..................................................................................... 36 2. MCNP Sample Input Deck for Gamma Spectroscopy ..................................................................... 36 3. Weight Measurements for Each Crucible and Salt Addition .......................................................... 40 4. MCNP Input Deck for Attenuation Correction .................................................................................... 41 5. Liquid Source Handling Procedure from OSURR Staff .................................................................... 45 vi List of Figures Figure 1: Electrorefiner schematic showing the separation of uranium, Major Actinides, and Fission Products in LiCl-KCl Eutectic Salt ................................................................................................................... 2 Figure 2: Na22 activity vs LiCl-KCl eutectic salt mass from [14]. .................................................................... 6 Figure 3: OSURR staff pipetting liquid source for addition to a crucible [14]. ........................................... 10 Figure 4: Spectral readout from the OSURR GRSS, with isotopic markers manually placed...................... 11 Figure 5: Glassy carbon crucible containing melted LiCl-KCl eutectic salt and added isotopes. ................ 11 Figure 6: Molten salt casting from the miniature waffle maker ................................................................. 12 Figure 7: Alumina crucible, with 5g of salt, on GRSS platform with a single Cs-137 button source. ........
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