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Cyclotron Production of Technetium-99m Open Access


Other title
Medical isotopes
Isotope shortage
Cyclotron production of technetium
Type of item
Degree grantor
University of Alberta
Author or creator
Gagnon, Katherine M
Supervisor and department
McQuarrie, S.A. (Oncology)
Robinson, D. (Oncology, Physics)
Examining committee member and department
Jans, H. (Oncology)
Mercer, J. (Oncology)
Lewis, J. (Radiology)
Krauss, C. (Physics)
Wilson, J. (Oncology)
Department of Physics
Medical Physics
Date accepted
Graduation date
Doctor of Philosophy
Degree level
Technetium-99m (99mTc) has emerged as the most widely used radionuclide in medicine and is currently obtained from a 99Mo/99mTc generator system. At present, there are only a handful of ageing reactors worldwide capable of producing large quantities of the parent isotope, 99Mo, and owing to the ever growing shutdown periods for maintenance and repair of these ageing reactors, the reliable supply 99mTc has been compromised in recent years. With an interest in alternative strategies for producing this key medical isotope, this thesis focuses on several technical challenges related to the direct cyclotron production of 99mTc via the 100Mo(p,2n)99mTc reaction. In addition to evaluating the 100Mo(p,2n)99mTc and 100Mo(p,x)99Mo reactions, this work presented the first experimental evaluation of the 100Mo(p,2n)99gTc excitation function in the range of 8–18 MeV. Thick target calculations suggested that large quantities of cyclotron-produced 99mTc may be possible. For example, a 6 hr irradiation at 500 μA with an energy window of 18 to 10 MeV is expected to yield 1.15 TBq of 99mTc. The level of coproduced 99gTc contaminant was found to be on par with the current 99Mo/99mTc generator standard eluted with a 24 hr frequency. Highly enriched 100Mo was required as the target material for 99mTc production and a process for recycling of this expensive material is presented. An 87% recovery yield is reported, including metallic target preparation, irradiation, 99mTc extraction, molybdate isolation, and finally hydrogen reduction to the metal. Further improvements are expected with additional optimization experiments. A method for forming structurally stable metallic molybdenum targets has also been developed. These targets are capable of withstanding more than a kilowatt of beam power and the reliable production and extraction of Curie quantities of 99mTc has been demonstrated. With the end-goal of using the cyclotron-produced 99mTc clinically, the quality of the cyclotron-produced 99mTc has been extensively compared with relevant United States Pharmacopeia (USP) specifications for the existing 99Mo/99mTc production strategy. Additional quality testing, including biodistribution studies of [99mTc]pertechnetate and [99mTc]disofenin in both mice and rabbits was also evaluated. Using the strategies and results presented throughout this dissertation, this thesis concludes with the world’s first cyclotron-based 99mTc patient images obtained as part of a Phase I Clinical Trial at the University of Alberta using [99mTc]pertechnetate.
Permission is hereby granted to the University of Alberta Libraries to reproduce single copies of this thesis and to lend or sell such copies for private, scholarly or scientific research purposes only. Where the thesis is converted to, or otherwise made available in digital form, the University of Alberta will advise potential users of the thesis of these terms. The author reserves all other publication and other rights in association with the copyright in the thesis and, except as herein before provided, neither the thesis nor any substantial portion thereof may be printed or otherwise reproduced in any material form whatsoever without the author's prior written permission.
Citation for previous publication
Chapter 2 A version of this chapter was published as a section in: K. Gagnon, S. McQuarrie, D. Abrams, A. J. B. McEwan and F. Wuest, Radiotracers based on technetium-94m, Current Radiopharmaceuticals, 4 (2011) 90–101.Chapter 3 A version of this chapter was published in: K. Gagnon, F. Bénard, M. Kovacs, T.J. Ruth, P. Schaffer, J.S. Wilson and S.A. McQuarrie, Cyclotron production of 99mTc: Experimental measurement of the 100Mo(p,x)99Mo, 99mTc, and 99gTc excitation functions from 8 to 18 MeV, Nucl. Med. Biol. 38 (2011) 907–916.Chapter 4 A version of this chapter was published in: K. Gagnon, M. Jensen, H. Thisgaard, J. Publicover, S. Lapi, S.A. McQuarrie, and T.J. Ruth, A new and simple calibration-independent method for measuring the beam energy of a cyclotron, Appl. Radiat. Isot. 69 (2011) 247–253.Chapter 5 A version of this chapter was submitted for review in: K. Gagnon, J. S. Wilson, C. Holt, D. Abrams, A. J. B. McEwan, D. Mitlin, and S.A. McQuarrie, Cyclotron production of 99mTc: Recycling of enriched 100Mo metal targets, submitted to Applied Radiation and Isotopes (August, 2011).Chapter 6 A version of this chapter was presented at the 19th International Symposium of Radiopharmaceuticals Sciences, Amsterdam, Aug 28th–Sept 2nd, 2011: K. Gagnon, C. Holt, J.S. Wilson, D. Mitlin, S. McQuarrie, Target preparation and recycling of molybdenum for the cyclotron production of 99mTc, J. Label. Compd. Radiopharm. 54 (2011) S54.Chapter 7 A version of this chapter was presented at the Annual Congress of the European Association of Nuclear Medicine, Birmingham, UK, October 15–19, 2011. K. Gagnon, D. Abrams, J.S. Wilson, S.A. McQuarrie, A.J.B. McEwan, Quality control of cyclotron vs. generator 99mTc-labeled radiopharmaceuticals, Eur. J. Nucl. Med. Mol. Imaging. 38 (2011), S105.

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