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(12) Patent Application Publication (10) Pub. No.: US 2013/0301769 A1 Schaffer Et Al

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(12) Patent Application Publication (10) Pub. No.: US 2013/0301769 A1 Schaffer Et Al US 2013 0301769A1 (19) United States (12) Patent Application Publication (10) Pub. No.: US 2013/0301769 A1 Schaffer et al. (43) Pub. Date: Nov. 14, 2013 (54) PROCESSES, SYSTEMS, AND APPARATUS Publication Classification FORCYCLOTRON PRODUCTION OF TECHNETUM-99M (51) Int. Cl. G2G I/00 (2006.01) (71) Applicant: TRIUMF, (US) C2.5D 13/02 (2006.01) (52) U.S. Cl. (72) Inventors: Paul Schaffer, Richmond (CA): CPC ................ G21G I/001 (2013.01); C25D 13/02 Francois Benard, Vancouver (CA); (2013.01) Kenneth R. Buckley, Vancouver (CA); USPC .............................. 376/195; 75/365; 204/507 Victoire Hanemaayer, Richmond (CA); Cornelia Hoehr Manuela, Vancouver (57) ABSTRACT (CA); Julius Alexander Klug, A process for producing technetium-99m from a molybde Vancouver (CA); Michael S. Kovacs, num-100 metal powder, comprising the steps of London (CA); Thomas J. Morley, New (i) irradiating in a Substantially oxygen-free environment, a Haven, CT (US); Thomas J. Ruth, hardened sintered target plate coated with a Mo-100 Vancouver (CA); John Valliant, metal, with protons produced by a cyclotron; Ancaster (CA); Stefan K. Zeisler, (ii) dissolving molybdenum ions and technetium ions from Vancouver (CA); Maurice G. Dodd, the irradiated target plate with an HO solution to form Vancouver (CA) an oxide solution; (iv) raising the pH of the oxide solution to about 14: (73) Assignee: TRIUMF, Vancouver (CA) (V) flowing the pH-adjusted oxide solution through a resin (21) Appl. No.: 13/870,830 column to immobilize KTcO ions thereon and to elute KMoO ions therefrom: (vi) eluting the bound KTcO ions from the resin column; (22) Filed: Apr. 25, 2013 (vii) flowing the eluted KTcO ions through an alumina column to immobilize KTcO ions thereon; Related U.S. Application Data (viii) washing the immobilized KTcO ions with water; (60) Provisional application No. 61/639,408, filed on Apr. (ix) eluting the immobilized KTcO ions with a saline 27, 2012, provisional application No. 61/640,610, Solution; and filed on Apr. 30, 2012. (x) recovering the eluted Na TcO ions. Natural Raw raterials molybdenum Stable isotope isolation High-purity Ho-100 feedstock Target plate O-100 fabrication Target plate Irradiation Protor irradiation Tatia Mo(p,2n) Mo-100 Recycling with 6-week cool-down period irradiated MO-100-)c-99m targets Primary Chemical Low-level processing extraction Waste Secondary cGMP processing chemistry Medical isotope distribution Patent Application Publication Nov. 14, 2013 Sheet 1 of 29 US 2013/0301769 A1 Natural RaW materials molybdenum Stable isotope isolation High-purity Mo-100 feedstock Target plate Mo-1 OO fabrication Target plate Irradiation Prote gton MO-100 p, Recycling with 6-week Cool-down period Irradiated MO-100 YTC-99m targets Primary Chemical LOW-level processing extraction Waste Secondary CGMP processing chemistry Medical isotope distribution Patent Application Publication Nov. 14, 2013 Sheet 2 of 29 US 2013/0301769 A1 •æææææææ),„ Patent Application Publication Nov. 14, 2013 Sheet 3 of 29 US 2013/0301769 A1 Patent Application Publication Nov. 14, 2013 Sheet 4 of 29 US 2013/0301769 A1 Patent Application Publication Nov. 14, 2013 Sheet 5 of 29 US 2013/0301769 A1 Patent Application Publication Nov. 14, 2013 Sheet 6 of 29 US 2013/0301769 A1 ZZ egzí !}}ZzZzZzZzZzZzZzZzzzzzzzz&? 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Patent Application Publication Nov. 14, 2013 Sheet 29 of 29 US 2013/0301769 A1 415 455 US 2013/0301769 A1 Nov. 14, 2013 PROCESSES, SYSTEMS, AND APPARATUS used, or Sodium pertechnetate can be used directly without FORCYCLOTRON PRODUCTION OF pharmaceutical tagging for specific procedures requiring TECHNETUM-99M only the Tc-99 mO as the primary radiopharmaceutical. 0004. The problem with fission-based production of TECHNICAL FIELD Tc-99m is that the several nuclear reactors producing the world-wide supply of Mo-99 are close to the end of their 0001. The present disclosure pertains to processes, sys lifetimes. Almost two-thirds of the world's supply of Mo-99 tems, and apparatus, for production of technetium-99m. currently comes from two reactors: (i) the National Research More particularly, the present pertains to production of tech Universal Reactor at the Chalk River Laboratories in Ontario, netium-99m from molybdenum-100 using accelerators such Canada, and (ii) the Petten nuclear reactor in the Netherlands. as cyclotrons. Both facilities were shut-down for extended periods of time in 2009-2010 which caused a serious on-going world-wide BACKGROUND shortage of supply of Mo-99 for medical facilities. Although 0002 Technetium-99m, referred to hereinafter as Tc-99m, both facilities are now active again, significant concerns is one of the most widely used radioactive tracers in nuclear remain regarding reliable long-term supply of Mo-99. medicine diagnostic procedures. Tc-99m emits readily 0005. It is known that medical cyclotrons can produce detectable 140 keV gamma rays and has a half-life of only small amounts of Tc-99m from Mo-100 for research pur about six hours, thereby limiting patients’ exposure to radio poses. It has been recently demonstrated that Tc-99m pro activity. Depending on the type of nuclear medicine proce duced in a cyclotron is equivalent to nuclear Tc-99m when dure, Tc-99m is bound to a selected pharmaceutical that used for nuclear medical imaging (Guerinet al., 2010, Cyclo transports the Tc-99m to its required location which is then tron production of'." Tc. An approach to the medical iso imaged by radiology equipment. Common nuclear medical tope crisis. J. Nucl. Med. 51(4): 13N-16N). However, analy diagnostic procedures include tagging Tc-99m to Sulfur col ses of numerous studies reporting conversion of Mo-100 to loids for imaging the liver, the spleen, and bone marrow, to Tc-99m show considerable discrepancies regarding conver macroaggregated albumin for lung Scanning, to phosphonates sion efficiencies, gamma ray production, and purity (Challan for bone scanning, to iminodiacetic acids for imaging the et al., 2007, Thin target yields and Empire-II predictions in hepatobiliary system, to glucoheptonates for renal scanning the accelerator production of technetium-99m. J. Nucl. Rad. and brain scanning, to diethylenetriaminepentaacetic acid Phys. 2:1-: Takacs et al., 2003, Evaluation of proton induced (DPTA) for brain scanning and kidney scanning, to dimer reactions on "Mo: New cross sections for production of captosuccinic acid (DMSA) for scanning the renal cortex, to "Tc and Mo. J. Radioanal. Nucl. Chem. 257: 195-201; red blood cells for blood pool scanning of the heart, to meth Lebeda et al., 2012, New measurement of excitation functions oxyisoburyl isonitrile (MIBI) for imaging myocardial perfu for (p,v) reactions on "Mo with special regard to the forma Sion, for cardiac ventriculography, and to pyrophosphate for tion of "Tc, "&Tc, "Te and Mo. Appl. Radiat. Isot. imaging calcium deposits in damaged hearts. Tc-99m is also 68(12): 2355-2365: Scholten et al., 1999, Excitation func very useful for detection of various forms of cancer for tions for the cyclotron production of "Tc and Mo. Appl. example, by identification of sentinal nodes, i.e., lymph nodes Radiat. Isot. 51:69-80). draining cancerous sites Such as breast cancer or malignant melanomas by first injecting a Tc-99m-labeled sulfur colloid SUMMARY OF THE DISCLOSURE followed by injection of a Tc-99m-labeled isosulfan blue dye. Immunoscintigraphy methods are particularly useful for 0006.
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