Investigation of Silver Nitrate–Impregnated Alumina As an Alternative Iodine Sorbent

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Investigation of Silver Nitrate–Impregnated Alumina As an Alternative Iodine Sorbent University of Tennessee, Knoxville TRACE: Tennessee Research and Creative Exchange Masters Theses Graduate School 12-2018 Investigation of Silver Nitrate–Impregnated Alumina as an Alternative Iodine Sorbent Jacob A. Jordan University of Tennessee Follow this and additional works at: https://trace.tennessee.edu/utk_gradthes Recommended Citation Jordan, Jacob A., "Investigation of Silver Nitrate–Impregnated Alumina as an Alternative Iodine Sorbent. " Master's Thesis, University of Tennessee, 2018. https://trace.tennessee.edu/utk_gradthes/5346 This Thesis is brought to you for free and open access by the Graduate School at TRACE: Tennessee Research and Creative Exchange. It has been accepted for inclusion in Masters Theses by an authorized administrator of TRACE: Tennessee Research and Creative Exchange. For more information, please contact [email protected]. To the Graduate Council: I am submitting herewith a thesis written by Jacob A. Jordan entitled "Investigation of Silver Nitrate–Impregnated Alumina as an Alternative Iodine Sorbent." I have examined the final electronic copy of this thesis for form and content and recommend that it be accepted in partial fulfillment of the equirr ements for the degree of Master of Science, with a major in Nuclear Engineering. Howard Hall, Major Professor We have read this thesis and recommend its acceptance: John D. Auxier II, Steven Skutnik Accepted for the Council: Dixie L. Thompson Vice Provost and Dean of the Graduate School (Original signatures are on file with official studentecor r ds.) Investigation of Silver Nitrate–Impregnated Alumina as an Alternative Iodine Sorbent A Thesis Presented for the Master of Science Degree The University of Tennessee, Knoxville Jacob A. Jordan December 2018 ACKNOWLEDGEMENTS This thesis was a collaborative effort with numerous people providing invaluable input. My thanks go out to UTK Professors Howard Hall, Steven Skutnik, and John Auxier II for graciously sitting on my committee and providing feedback throughout the process. I am indebted to Oak Ridge National Laboratory for providing facilities, research, and a job. At the lab, my co-workers Stephanie Bruffey, Joe Walker, and Barry Spencer were invaluable in providing support and knowledge as I stumbled my way around the lab. Bob Jubin deserves special mention for providing a project and extensive guidance as a true expert in the field. This work could not have been done without Rodney Hunt (ORNL) for providing testing material. I’m grateful to David Glasgow, Riley Hunley, and Justin Knowles for doing the neutron activation analysis required for this project at ORNL’s High Flux Isotope Reactor. Joseph Birdwell was immensely helpful in hiring me into the Process Engineering Group, supporting my work on this project, and being an encouraging group leader. I would also like to thank UTK Professor Jamie Coble for providing me my first research group home and vastly improving my computer skills. Lastly, and most importantly, I must thank my wife, Sarah, for being (very) patient during the publishing process. ii ABSTRACT United States regulations on nuclear reprocessing would limit the release of certain radioactive volatile species, including 3H, 14C, 85Kr, and 129I. Conservative analyses indicate that >99.9% of the iodine contained in used nuclear fuel could require capture. Solid sorbents for this application include silver mordenite (AgZ) and silver nitrate– impregnated alumina (AgA). AgA has been studied previously under simulated possible reprocessing conditions to assess its effectiveness as an iodine sorbent, and those results have been compared with well-characterized AgZ. To date, AgZ and AgA have been investigated for use in iodine capture from off- gas generated by aqueous fuel reprocessing. However, modifications to traditional reprocessing have been considered, including upfront tritium pretreatment using NO2 as the oxidant. This introduces large amounts of NO2 to the off-gas, which has been shown to severely degrade the iodine capture performance of AgZ. Literature regarding the behavior of AgA in NO2-bearing gas streams suggested that AgA could be better able to retain its iodine-capture capabilities under these high-NO2 conditions. This hypothesis was tested by exposing AgA to a high-NO2 environment for varying periods of time and then measuring the iodine capacity of the sorbent. AgA retained 85%, 65%, and 25% of its capture capacity when exposed to NO2 for 1 week, 2 weeks, and 4 weeks prior to testing, respectively. When aged for 1 week and 4 weeks, AgZ only retained 3% and 8% of its capture capacity. In non-oxidizing conditions, the capture performance of the sorbents is similar. Thus, this thesis supports the theory that AgA is more robust to the presence of NO2 than AgZ and merits further consideration if advanced tritium pretreatment is to be performed during fuel reprocessing. iii TABLE OF CONTENTS 1. Introduction .................................................................................................................. 1 Reprocessing and Off-Gas Basics ................................................................................. 3 Dose Limits and Off-gas Mitigation Requirements ........................................................ 5 Release Limits/Dose Regulations ............................................................................... 6 Decontamination Factor Requirements ...................................................................... 6 Iodine Behavior in Reprocessing Plant and Off-Gas ..................................................... 8 Head end processes (shearing and tritium pretreatment) ......................................... 8 Dissolver Off-Gas ........................................................................................................ 8 Vessel Off-Gas ............................................................................................................ 9 Summary of Iodine Off-Gas ...................................................................................... 10 2. Literature Review ...................................................................................................... 11 Historical Approaches to Iodine Capture ..................................................................... 11 AgA as iodine sorbent................................................................................................... 14 High NO2 Impact on Iodine Sorption ............................................................................ 17 Summary ....................................................................................................................... 20 3. Motivation and Proposed Research ......................................................................... 22 4. Methodology .............................................................................................................. 23 Sample Preparation ...................................................................................................... 23 System Setup and Design ............................................................................................ 24 Experimental Procedure ............................................................................................... 26 5. Analysis ..................................................................................................................... 27 Weight Estimates .......................................................................................................... 27 Neutron Activation Analysis .......................................................................................... 28 6. Results and Discussion ............................................................................................. 29 Concentration Series .................................................................................................... 29 Humidity Series ............................................................................................................. 30 Temperature Series ...................................................................................................... 30 NO2 Aging Series .......................................................................................................... 31 Water Loading, No Iodine ............................................................................................. 32 Error Analysis ................................................................................................................ 33 7. Conclusions ............................................................................................................... 37 8. Future Work ............................................................................................................... 40 Iodine Speciation .......................................................................................................... 40 Iodine Loading Form ..................................................................................................... 41 Determination of Experimental Error ............................................................................ 42 Works Cited ...................................................................................................................... 43 Appendix ........................................................................................................................... 47 Appendix A: Tables ....................................................................................................... 48 Appendix B:
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