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Non-Destructive, Near-Real-Time Nuclear Safeguards Monitoring at a Reprocessing Facility

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Non-Destructive, Near-Real-Time Nuclear Safeguards Monitoring at a Reprocessing Facility The Multi-Isotope Process Monitor: Non-destructive, Near-Real-Time Nuclear Safeguards Monitoring at a Reprocessing Facility Dissertation Presented in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy in the Graduate School of The Ohio State University By Christopher Robert Orton, M.S. Graduate Program in Nuclear Engineering The Ohio State University 2009 Dissertation Committee: Richard N. Christensen, Advisor Richard S. Denning Xiaodong Sun Abstract The IAEA will require advanced technologies to effectively safeguard nuclear material at envisioned large scale nuclear reprocessing plants. This dissertation describes results from simulations and experiments designed to test the Multi-Isotope Process (MIP) Monitor, a novel safeguards approach for process monitoring in reprocessing plants. The MIP Monitor combines the detection of intrinsic gamma ray signatures emitted from process solutions with multivariate analysis to detect off-normal conditions in process streams, nondestructively and in near-real time (NRT). Three different models were used to predict spent nuclear fuel composition, estimate chemical distribution during separation, and simulate spectra from a variety of gamma detectors in product and raffinate streams for processed fuel. This was done for fuel with various irradiation histories and under a variety of plant operating conditions. Experiments were performed to validate the results from the model. Three segments of commercial spent nuclear fuel with variations in burnup and cooling time were dissolved and subjected to a batch PUREX method to separate the uranium and plutonium from fission and activation products. Gamma spectra were recorded by high purity germanium (HPGe) and cadmium zinc telluride (CZT) detectors. Hierarchal Cluster Analysis (HCA) and Principal Component Analysis (PCA) were applied to spectra from both model and experiment to investigate spectral variations as a function of acid concentration, burnup ii level and cooling time. Partial Least Squares was utilized to extract quantitative information about process variables, such as acid concentration or burnup. The MIP Monitor was found to be sensitive to the induced variations of the process and was capable of extracting quantitative process information from the analyzed spectra. iii Dedication Dedicated to my wife, children and God May we, His children, use atomic power for peace and prosperity iv Acknowledgments There are many people that have helped in the completion of this dissertation to whom I am grateful. First, I want to thank my wife and children. Their love, support and patience have made this journey not only possible, but enjoyable. My successes are their successes and I am eternally grateful for their sacrifice. I appreciate the support of my parents and my wife’s parents. Their support has been constant and reassuring. I am also grateful for the support of our grandparents and the example of my father and grandfathers. Their lives have provided both inspiration and background for this dissertation. I wish to express my thanks and gratitude to my advisor, Dr. Richard Christensen. Thank you for the opportunity, the support, the advice, the patience, the guidance and ultimately the encouragement for this dissertation as well as life. I am extremely grateful to have had the opportunity to be instructed by you and to work with you. I also wish to thank Pamela Christensen for her support to me and also my family. We are grateful for the meals and the fun times. We’ve been uplifted by your service. I wish to express my thanks to my mentor and friend at Pacific Northwest National Laboratory, Dr. Jon Schwantes. Thank you for the project, the funding, and the education. More importantly, thank you for pushing me to perform better and for keeping your sense of humor. I appreciate the guidance and unwavering support. It has v been a privilege to complete my dissertation with you and I’m grateful for all you’ve done. I wish to thank the additional members of my committee: Dr. Richard Denning, Dr. Don Miller, Dr. Xiaodong Sun, and Steve Maheras. I thoroughly enjoyed my education at The Ohio State University due in large part to the efforts of these men. Thank you for your courses, instruction, and wise counsel. Your efforts have been invaluable and impactful. Thank you. I wish to thank my friends and associates at Pacific Northwest National Laboratory, including Matt Douglas, Amanda Johnsen, Sam Bryan, Tatiana Levitskaia, Chuck Soderquist, Lori Darnell, Leah Arrigo, Mark Englemann, Chris Aardahl (and everyone else in the Advance Radioanalytical Chemistry Group), Dan Couch, Andy Prichard, Mark Shaver, Richard Pagh, Chris Gesh, Ann Doherty, Jeremy Kephart, Larry Greenwood, Kathie Thomas, Walt Hensley, Shane Peper, Carrie Mathews, Brian W. Smith, Khris Olsen and Mark Killinger. All of you have made contributions, whether large or small to the successful completion of this work and also to my career path, education, and achievements at PNNL. I am grateful for your help. Finally I would like to thank the U.S. Department of Energy’s Fuel Cycle Research and Development program (formerly GNEP and AFCI) for their financial support of this project. Additional support for the experimental demonstrations was provided by the U.S. DOE’s NA-243 office. I would also like to thank Cathy Dixon and the AFCI fellowship program for additional financial support for my education and research. Though this work has been funded by the U.S. DOE, any opinions, findings, vi and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the Department of Energy. vii Vita 1998…………………………………………………………………Richland High School 2004-2007……………...National Security Intern, Pacific Northwest National Laboratory 2005………………………..........B.S. Chemical Engineering, Brigham Young University 2007……………………………….M.S. Nuclear Engineering, The Ohio State University 2008-Present….Post Masters Research Associate, Pacific Northwest National Laboratory Publications 1. C.R. Orton, D.Y. Parkinson, P.D. Evans, N.L. Owen, “Fourier Transform Infrared Studies of Heterogeneity, Photodegradation, and Lignin/Hemicellulose Ratios Within Hardwoods and Softwoods,” Applied Spectroscopy, Vol. 58, Num. 11, p. 1265-1271 (2004). 2. L.E. Smith, J.M. Schwantes, M. Douglas, J.J. Ressler, C. Durst, C.R. Orton, R.N. Christensen, “Next-Generation Online MC&A Technologies for Reprocessing Plants,” Global 2007: Advanced Fuel Cycles and Systems, September 13, Boise, ID (2007). 3. J.M. Schwantes, M. Douglas, C.R. Orton, C. Fraga and R.N. Christensen, “Multi- Isotope Process (MIP) Monitor: a Near-Real-Time Monitor for Reprocessing Facilities,” ANS Transactions from Annual Meeting, Anaheim, CA (2008). 4. C.R. Orton, J.M. Schwantes, S.A Bryan, T.G. Levitskaia, D.C. Duckworth, M. Douglas, O.T. Farmer, III, C.G. Fraga, S.A. Lehn, M. Liezers, S.M. Peper, and R.N. Christensen, “Advanced Safeguards Technology Demonstration at Pacific Northwest National Laboratory,” Conference Proceedings of the Institute of Nuclear Materials Management 49th Annual Meeting, Nashville, TN (2008). 5. J.M. Schwantes, M. Douglas, S. Bonde, J.D. Briggs, O.T. Farmer, L.R. Greenwood, E.A. Lepel, C.R. Orton, J.F. Wacker, A.T. Luksic, “Nuclear Archeology in a Bottle: viii Evidence of Pre-Trinity U.S. Weapons Activities from a Waste Burial Site,” Analytical Chemistry, Vol. 81, 4, p. 1297-1306 (2009). 6. M.A. Green, L.M. Arrigo, M. Liezers, C.R. Orton, M. Douglas, S.M. Peper, J.M. Schwantes, and D.C. Duckworth, “Electrochemically-Modulated Separations for Destructive and Nondestructive Analysis for Process Monitoring and Safeguards Measurements,” Institute of Nuclear Materials Management 50th Annual Meeting, Tucson, AZ (2009). 7. L.M. Arrigo, S.A. Bryan, R.N. Christensen, M. Douglas, D.C. Duckworth, C.G. Fraga, M. Liezers, C.R. Orton, S.M. Peper, and J.M. Schwantes, “Advanced Safeguards Technology Demonstration at Pacific Northwest National Laboratory,” Institute of Nuclear Materials Management 50th Annual Meeting, Tucson, AZ (2009). 8. J.M. Schwantes, C.R. Orton, C.G. Fraga, M. Douglas, and R.N. Christensen, “The Multi-Isotope Process (MIP) Monitor: a Near-Real-Time, Non-Destructive, Indicator of Spent Nuclear Fuel Reprocessing Conditions,” Institute of Nuclear Materials Management 50th Annual Meeting, Tucson, AZ (2009). 9. C.R. Orton, J.M. Schwantes, C.G. Fraga, M. Douglas, and R. Christensen, "Experimental Validation of the Multi-Isotope Process Monitor Concept," Conference Proceedings of GLOBAL 2009 "The Nuclear Fuel Cycle: Sustainable Options & Industrial Perspectives" September 6-11, 2009, Paris, France (2009). Fields of Study Major Field: Nuclear Engineering ix Table of Contents Abstract .......................................................................................................................... ii Dedication ..................................................................................................................... iv Acknowledgments ...........................................................................................................v Vita ............................................................................................................................. viii List of Tables................................................................................................................ xii List of Figures ............................................................................................................. xiii Chapter
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