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Mo-99 Tc-99M Supporting Material Final report of the coordinated research project On Accelerator-based Alternatives to Non-HEU Production of Mo-99 /Tc-99m 1 EDITORIAL NOTE This publication has been prepared from the original material as submitted by the authors. The views expressed do not necessarily reflect those of the IAEA, the governments of the nominating Member States or the nominating organizations. The use of particular designations of countries or territories does not imply any judgments by the publisher, the IAEA, as to the legal status of such countries or territories, of their authorities and institutions or of the delimitation of their boundaries. The mention of names of specific companies or products (whether or not indicated as registered) does not imply any intention to infringe proprietary rights, nor should it be construed as an endorsement or recommendation on the part of the IAEA. The authors are responsible for having obtained the necessary permission for the IAEA to reproduce, translate or use material from sources already protected by copyrights. 2 Table of Contents SUMMARY .................................................................................................................................................................. 5 REPORTS BY THE PARTICIPANTS OF THE COORDINATED RESEARCH PROJECT ................................... 15 TECHNOLOGY DEVELOPMENT FOR 99MTC DIRECT PRODUCTION UNDER PROTON BEAM FROM C18 CYCLOTRON AT NATIONAL SCIENCE LABORATORY ........................................................................... 16 A. Avetisyan, R. Dallakyan, R. Sarkisyan, A. Melkonyan, M. Mkrtchyan, G. Harutyunyan, N. Dobrovolsky, S. Sergeeva ACCELERATOR-BASED ALTERNATIVES TO NON-HEU PRODUCTION OF 99Mo/99mTc ............................. 31 S.A. Mcquarrie, K. Gagnon, J. Andersson, J. Wilson, E. Schirrmacher, B. Thomas, R. Lecomtb, S. Selivanob, H. Senta, B. Guérin, E. Turcotte, A. Zyuzin and A.J.B. Mcewan A COMPLETE SOLUTION TO PRODUCING 99MTC VIA PROTON BOMBARDMENT OF 100MO ................... 52 thomas J. Ruth NUCLEAR DATA FOR ACCELERATOR PRODUCTION OF 99MTC ................................................................... 69 s. Takacs CYCLOTRON PRODUCTION OF 99mTc AND DEVELOPMENT OF A NEW METHOD OF SEPARATION 99M - OF TcO4 FROM THE IRRADIATED MOLYBDENUM TARGET ................................................................... 91 malay Kanti Dasa, Madhusmitaa, Sankha Chattopadhyaya, Sujata Saha Dasa, Md. Nayer Alama, Luna Baruaa, Anirban Deb, Umesh Kumara, Siddhartha Dattac ACCELERATOR-BASED ALTERNATIVES TO NON-HEU PRODUCTION OF Tc-99m ................................. 110 J. Espositoa, M. Bellob, A. Boschic,D, G. Cicoriae ,L. De Nardob G. Di Domenicod, A. Duattif, M. Gambaccinib, M. Gigantic, L. Ginig, F. Groppig, U. Holzwarthh, M. Loriggiolaa G. Lucconie, S. Manentig, M. Marengoe, P. Martinia,B,, L. Melendez-Alaforti, A. Negrij, V. Palmieria, M. Pasqualic,D, G. Pupilloa,D A. Rostatoi, A. Rossia H. Skliarovaa, A. Taibid, L. Uccellic,K, N. Uzunovl 99mTc PRODUCTION BY 18MEV PROTONS ON 100Mo TARGET: RESULTS AND CONSIDERATIONS ...... 110 M. Clemenzacd, F. Groppif, S. Manentif, M. Oddoneb,E, A. Salvinia,E, L. Stradaa,E EVALUATION OF THE 99mTc REMOTE PRODUCTION BY PROTON BOMBARDMENT ON 100Mo TARGET ................................................................................................................................................................... 142 Kotaro Nagatsua, Keiko Tagamib, Toshimitsu Fukumuraa, Shigeo Uchidab, Yasuhisa Fujibayashia CYCLOTRON PRODUCTION OF 99mTc - COLLABORATIVE PROJECT IN POLAND ................................... 155 R. Mikołajczaka, J.L. Parusa, D. Pawlaka, T. Janiaka, W. Wojdowskaa, I. Cieszykowskaa, K. Jerzyka, P. Garnuszeka, M. Mielcarskia, J. Choińskib, J. Jastrzębskib, A. Stolarzb, A. Trzcińskab, A. Bilewiczc, M. Gumielac, E. Gniazdowskac, P. Koźmińskic, K. Szkliniarzd,W. Zipperd PRODUCTION OF TC-99M AT KING FAISAL SPECIALIST HOSPITAL AND RESEARCH CENTRE (KFSHRC) ................................................................................................................................................................ 175 I. Al-Jammaza, F. Al-Rumayana, S. Al-Yanbawia, And A. Al-Rabihaa HIGH ACTIVITY CYCLOTRON PRODUCED TC-99M FOR MEDICAL APPLICATIONS ............................. 175 Al Rayyes A. H. 3 CYCLOTRON PRODUCTION OF 99mTc AND 186Re AT WASHINGTON UNIVERSITY .................................. 199 Vernal Richards And Suzanne E. Lapi LIST OF CRP PARTICIPANTS .............................................................................................................................. 212 4 SUMMARY 1. INTRODUCTION A number of IAEA Member States have embarked on research programs to investigate the use of accelerators for the production of Mo-99 or Tc-99m directly. These approaches make use of the 100Mo(γ,n)99Mo and 100Mo(p,2n)99mTc reactions, respectively. While the photo transmutation of Mo-100 is based on solid scientific evidence, the actual implementation of this approach will involve development in the area of high power electron machines of suitable energy (25-40 MeV) and technological advances in the electron converter. In 100Mo(p,2n)99mTc reaction approach, there is an issue on the purity of the final Tc- 99m product both from the isotopic ratio of the molybdenum starting material and the proton energy and the ΔE for the particular target. In addition, the isotopic composition for an enriched target will affect the radionuclidic composition of the target matrix. There are several approaches to isolating and purifying the Tc-99m extracted from the target material. A more complete understanding regarding reproducibility, purity and efficiency for these approaches is needed using prescribed metrics for direct comparisons. The impact of specific activity (Tc-99m/all Tc isotopes including Tc-99g) has to be determined in order to define the shelf-life of the accelerator produced Tc-99m in comparison to generator produced Tc-99m in the formulation of radiopharmaceutical kits. The stability of the isolated Tc-99m pertechnetate solution as a function of time and the stability of the prepared radiopharmaceutical will affect the shelf life of the product. The path to recovery of the enriched Mo-100 target material involves tracking the isotopic composition and chemical/radionuclidic impurities. 1.1. Potential areas proposed for Coordinated Research Potential areas of further investigations were: The impact of Tc-99g and other Tc-isotopes on radiopharmaceutical labelling efficiency and consequence on image quality. How much Tc-99g and other Tc- isotopes will be produced, and how can these impurities be minimized if necessary? Measurement of still missing data which need to be determined for the large-scale accelerator-based production of 99mTc. Procedures for preparation of an isotopically enriched molybdenum accelerator target. Methods to recover pertechnetate from molybdenum accelerator targets post- irradiation. Quality Control (QC) parameters required for evaluation of radiopharmaceuticals prepared with cyclotron-produced pertechnetate. Recycling methods to recover enriched Mo from irradiated targets, as well as the impact of recycling enriched Mo on the quality of Tc-99m. 5 2. CRP OVERALL OBJECTIVE The overall objective of this CRP is the development of procedures on accelerator based production of Molybdenum-99/Technetium-99m with emphasis on development and optimization of production methods of Tc-99m via the (p,2n) reaction. 2.1. Specific Research Objective To determine: Radionuclide production profiles at various beam energies and intervals. Manufacturing of robust 100Mo accelerator target. Automated Mo/Tc separation system and chemical impurity profile. Labelling efficiency and image quality of Tc-radiopharmaceuticals using cyclotron- produced 99mTc. Dosimetry and its impact on shelf life Recycling of 100Mo and assessment of the effects of isotopic composition. 2.2. Salient Aspects of the CRP The participants of the CRP concluded that the project has helped to exchange valuable information and to become acquainted with other laboratories’ approaches and procedures and has stimulated cooperation between participating institutions as well as with relevant national counterparts. The specific objectives pursued by the CRP participants varied from country to country subject to the research priorities defined by the national teams, but the overall objectives of the CRP are well addressed. 3. SUMMARY OF THE WORK DONE IN CRP PARTICIPATING INSTITUTIONS 3.1. ARMENIA: National Science Laboratory (Yerevan Physics Institute) Foundation The activities of target preparation technology, target module cryogenic cooling system design, chemical separation and recovery of target material have been performed. A new technology of molybdenum target preparation using solid state laser focusing beam processing to the front of tablet has been created and tested. The molybdenum powder is melted in trace of laser, creating a solid strip of molybdenum with a width of a few hundred micrometers. The laser beam applying to press-fitted Mo tablet increased the mechanical strength and its thermal conductivity. For 99mTc extraction from the irradiated Mo a centrifuge extractor with Methyl Ethyl Ketone (MEK) solvent technology was chosen. The irradiated Mo oxidized in H2O2 peroxide, then dissolved in KOH alkali and then MEK liquid is added to that solution. The irradiated Mo dissolves in KOH while 99mTc dissolves in MEK so that we have mixture of two solutions with very different
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