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Production Potential of Scandium-47 Using Spallation Neutrons at Los Alamos Isotope Production Facility

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Production Potential of Scandium-47 Using Spallation Neutrons at Los Alamos Isotope Production Facility Air Force Institute of Technology AFIT Scholar Theses and Dissertations Student Graduate Works 3-14-2014 Production Potential of Scandium-47 Using Spallation Neutrons at Los Alamos Isotope Production Facility Kerriann A. DeLorme Follow this and additional works at: https://scholar.afit.edu/etd Recommended Citation DeLorme, Kerriann A., "Production Potential of Scandium-47 Using Spallation Neutrons at Los Alamos Isotope Production Facility" (2014). Theses and Dissertations. 644. https://scholar.afit.edu/etd/644 This Thesis is brought to you for free and open access by the Student Graduate Works at AFIT Scholar. It has been accepted for inclusion in Theses and Dissertations by an authorized administrator of AFIT Scholar. For more information, please contact [email protected]. PRODUCTION POTENTIAL OF 47Sc USING SPALLATION NEUTRON FLUX AT THE LOS ALAMOS ISOTOPE PRODUCTION FACILITY THESIS K. Austin DeLorme, 1st Lieutenant, United States Air Force AFIT-ENP-14-M-02 DEPARTMENT OF THE AIR FORCE AIR UNIVERSITY AIR FORCE INSTITUTE OF TECHNOLOGY Wright-Patterson Air Force Base, Ohio DISTRIBUTION STATEMENT A APPROVED FOR PUBLIC RELEASE; DISTRIBUTION UNLIMITED The views expressed in this document are those of the author and do not reflect the official policy or position of the United States Air Force, the United States Department of Defense or the United States Government. This material is declared a work of the U.S. Government and is not subject to copyright protection in the United States. AFIT-ENP-14-M-02 PRODUCTION POTENTIAL OF 47Sc USING SPALLATION NEUTRON FLUX AT THE LOS ALAMOS ISOTOPE PRODUCTION FACILITY THESIS Presented to the Faculty Department of Engineering Physics Graduate School of Engineering and Management Air Force Institute of Technology Air University Air Education and Training Command in Partial Fulfillment of the Requirements for the Degree of Master of Science K. Austin DeLorme, BS 1st Lieutenant, United States Air Force March 2014 DISTRIBUTION STATEMENT A APPROVED FOR PUBLIC RELEASE; DISTRIBUTION UNLIMITED AFIT-ENP-14-M-02 PRODUCTION POTENTIAL OF 47SC USING SPALLATION NEUTRON FLUX AT THE LOS ALAMOS ISOTOPE PRODUCTION FACILITY K. Austin DeLorme, BS 1st Lieutenant, United States Air Force Approved: //signed// 6 March 2014 Maj Benjamin Kowash, PhD (Chairman) Date //signed// 14 March 2014 LTC Stephen McHale, PhD (Member) Date //signed// 10 March 2014 Dr. Jonathan Engle, PhD (Member) Date //signed// 14 March 2014 Dr. Justin Clinton, PhD (Member) Date AFIT-ENP-14-M-02 Abstract Scandium-47 (T1=2 = 3:41d) forms stable complexes with aminopolycarboxylic acids, such as folate conjugates, which are useful as tumor biomarkers or antigens. Its thera- peutic beta emissions at 441.1 keV (Eβ−;max,Iβ− = 68%) and 600.5 keVmax (Eβ−;max,Iβ− = 32%) are coupled with an imageable 159.4 keV gamma to permit in vivo-tracking of compound biodistribution. Currently, its wider clinical application is hindered by lack of availability, even as interest grows in radioscandium-based pharmaceuticals thanks 44 to the successful development of Sc (94.27% β+; T1=2 = 3:97h) imaging agents. We have investigated the 47Ti(n,np) 47Sc, 50Ti(n,3p) 47Sc,natV(n,x)47Sc, and natTi(n,x)47Sc reactions as potential routes to therapeutically relevant quantities of 47Sc. Targets of natV, natTi, and enriched 47Ti (95.7% isotopic abundance) and 50Ti (83.1%) oxide targets were exposed to the spallation neutrons resulting from the proton-irradiation of RbCl and Ga targets at the Los Alamos National Laboratory (LANL) Isotope Production Facility (IPF). Targets were activated for 1 hr using an average proton beam current of 218±14 µAh incident on IPF targets. Derived production rates for 47Sc, expressed as activity created per gram of target material and per Ah of incident proton beam, are 0.146±.005 µCi g−1 µAh−1 in the natV foil, 0.44±0.01 µCi g−1 µAh−1 in the natTi foil, and 0.21±0.09 µCi g−1 µAh−1 and 0.34±0.2 µCi g−1 µAh−1 in the 47Ti and 50Ti-oxide samples, respectively. Radioisotopic purities of 47Sc in excess of 90% are achieved by activation of 47Ti targets, and small yields of 47Ca produce 47Sc with 100% radioiso- topic purity from activation of 50Ti. Yields and neutron fluxes predicted by MCNP6 event generators and evaluated nuclear data are also compared with the results of these activation experiments. iv AFIT-ENP-14-M-02 Dedicated to the SlaughterHaus. Thanks. 1 Acknowledgements As with anything, this work was the product of a lot of effort and assistance from many wonderful people I was fortunate enough to interact with throughout this process. I'd like to start by acknowledging Col John Weidner, my initial advisor whom introduced me to the Isotope Production Facility and opened the door to this great opportunity. I would also like to thank Maj Benjamin Kowash for taking on my project, despite its peculiarity in the AFIT setting, and for his assistance along the way. This goes, as well, to my AFIT committee members, LTC Stephen McHale, and Dr. Justin Clinton. I would like to give a special thank you to Dr. Jon Engle for all of his time, effort and the exceptional mentorship he provided me with throughout this entire process. The patience and time commitment he put into working with me was beyond my expecta- tions. I'm exceedingly grateful for his persistently thoughtful responses to every phone call and email, as I flooded his inbox regularly. Along with Jon, I would like to acknowledge the entirety of the Inorganic, Isotope and Actinide Chemistry (C-IIAC) Division at Los Alamos. Meiring Nortier also took a great deal of time to mentor and assist this effort. It was an honor to be able to learn from Meiring's knowledge and vast experience in the field. Dr. Eva Birnbaum was an invaluable asset both programmatically and academically{this experiment would have never gone forward without her efforts. The same may be said for Dr. Kevin John whose oversight ensured the project was properly supported. There are several individuals at Los Alamos who were invaluable to the experimental process. Wayne Taylor who kept three young physicists from causing too much chaos in our attempts to do black magic (a.k.a. chemistry), and who consistently offered his experience and assistance. Lauren Marus, who spent hours carefully measuring and preparing samples, as well as working on numerous other parts of the experiment. As well, Dr. Kevin Jackman who manned the count room and ensured data was properly 2 and accurately acquired and provided. Additionally I'd like to thank Dr. Hong Bach, Dave Reass and Michael Connors for their assistance at IPF during preparation, irradiation and target transport. I'd like to acknowledge Luke Daemen for his assistance in mentorship in the art of blowing glass, as well as Art and Dave in the machine shop. I'd also like to thank the entire crew of the Hot Cell Laboratory for all of their efforts. There were numerous other individuals with whom I interacted while in Los Alamos { as a whole, thank you for your time, assistance and kindness. I would like to thank my older brother, for pausing his life every time I called to help mediate my relationship with my computer. Finally I would like to acknowledge my entire wonderful family for their continued love and support. Last but not least, I need to extend a special thank you to the Slaughters for every- thing they have done for me over the last year and a half{from late night talks about "what could possibly be making a mess of these peaks!" to yogurt dates when one more MCNP error would have sent me over the edge. It's a blessing to have a family away from home. There are never enough words to catch it all - so I'll conclude with a simple, "Thanks." K. Austin DeLorme 3 Table of Contents Page Abstract . iv Acknowledgements . .2 List of Figures . .5 List of Tables . .6 1. Introduction . .1 1.1 Background . .1 1.1.1 Scandium-47 . .2 1.2 Research Objective . .3 1.3 Summary . .3 2. Theory...............................................................4 2.0.1 Radioactive Isotopes in Medicine . .4 2.0.2 Dual Purpose Theragnostic Radionuclides . .6 2.1 The Isotope Production Facility . .7 2.1.1 Spallation Neutron Flux at IPF . .9 2.2 Published Production Methods and Results . 10 2.2.1 Efforts at Brookhaven National Laboratory . 11 2.2.2 Other 47T i(n; p) Experiments . 12 2.2.3 Other Efforts . 13 3. Modeling Approach . 14 3.1 Neutron Flux Characterization . 14 3.1.1 MCNP6 . 14 3.1.2 Physics Models . 16 3.1.3 MCNP Flux Tallies . 19 3.1.4 Neutron Flux Model . 20 3.1.5 Variance Reduction . 20 3.1.6 Modeled Neutron Flux . 21 3.2 Modeled Yield Prediction . 23 3.2.1 Cinder90 . 23 3.2.2 MCNP Residual Nuclide Tally . 37 3.2.3 Cross Section Derivation . 39 3.2.4 MCNP Yield Estimation . 40 4 Page 4. Experimental Technique . 47 4.1 Target Preparation . 47 4.1.1 Oxide Powder Preparation . 48 4.1.2 Foil Target Preparation . 50 4.2 Irradiation . 52 4.3 Sample Transport . 54 4.4 Counting Preparation of Foil Samples . 55 4.5 Counting Preparation of Oxide Samples . 57 4.6 Gamma Counting . 60 5. Results and Analysis . 63 5.1 Count room Spectroscopy . 63 5.2 Decay Analysis Method . 65 5.2.1 Weighted Linear Least Squares Fit . 66 5.3 Peak Fit Results . 68 5.4 Radiochemical Loss in Oxide Dilution . 76 5.4.1 Peak Analysis of Counter 77 Data . 78 5.5 Experimental Production Rates .
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