The fundamentals of 99mTc production cycle at electron accelerator

The report presents the results of investigations into physical and technological fundamentals of 99Mo/99mTc production with the use of bremsstrahlung of the electron accelerator. Викладені результати розробки фізичних і технологічних основ виробництва 99Мо/99mТс із використанням гальмівного випром...

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Опубліковано в: :Вопросы атомной науки и техники
Дата:2004
Автори: Dikiy, N.P., Dovbnya, A.N., Uvarov, V.L.
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Опубліковано: Національний науковий центр «Харківський фізико-технічний інститут» НАН України 2004
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Цитувати:The fundamentals of 99mTc production cycle at electron accelerator / N.P. Dikiy, A.N. Dovbnya, V.L. Uvarov // Вопросы атомной науки и техники. — 2004. — № 1. — С. 168-171. — Бібліогр.: 8 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
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author Dikiy, N.P.
Dovbnya, A.N.
Uvarov, V.L.
author_facet Dikiy, N.P.
Dovbnya, A.N.
Uvarov, V.L.
citation_txt The fundamentals of 99mTc production cycle at electron accelerator / N.P. Dikiy, A.N. Dovbnya, V.L. Uvarov // Вопросы атомной науки и техники. — 2004. — № 1. — С. 168-171. — Бібліогр.: 8 назв. — англ.
collection DSpace DC
container_title Вопросы атомной науки и техники
description The report presents the results of investigations into physical and technological fundamentals of 99Mo/99mTc production with the use of bremsstrahlung of the electron accelerator. Викладені результати розробки фізичних і технологічних основ виробництва 99Мо/99mТс із використанням гальмівного випромінювання прискорювача електронів. Изложены результаты разработки физических и технологических основ производства 99Мо/99mТс с ис- пользованием тормозного излучения ускорителя электронов.
first_indexed 2025-12-01T03:58:19Z
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fulltext BEAM APPLICATIONS THE FUNDAMENTALS OF 99mTc PRODUCTION CYCLE AT ELECTRON ACCELERATOR N.P. Dikiy, A.N. Dovbnya, V.L. Uvarov National Science Center “Kharkov Institute of Physics and Technology”, 61108, Kharkov, Ukraine; E-mail: uvarov@kipt.kharkov.ua The report presents the results of investigations into physical and technological fundamentals of 99Mo/99mTc pro- duction with the use of bremsstrahlung of the electron accelerator. PACS: 06.60.Mr, 07.85.-m, 07.88+y, 81.30.Hd, 81.70.Jb 1. INTRODUCTION 99mTc (daughter nucleus of 99Mo) is the basic ra- dionuclide used in the present-day medical diagnostics. The main part of 99Mo is produced in nuclear reactors with the use of the 235U fission reaction [1]. The special features of 99Mo/99mTc generation at the electron acceler- ator are determined by both a low production cross-sec- tion for this isotope in photonuclear reactions (~180 mbn) and a great transport length of high-energy photons in substance. These special features set the re- quirements on the systems of initial electron beam for- mation and control, beam conversion into the bremsstrahlung flux, on the target device and beam pa- rameter monitoring in the process of irradiation, and also on the system of radiochemical extraction of 99mTc from the target. So, while the specific activity of fission- produced 99Mo reaches 103 Ci/g [1], in the electron ac- celerator case, this parameter makes ~0.1 Ci/g for the natural molybdenum target and ~1 Ci/g for the target enriched in the 100Mo isotope. This circumstance re- stricts the choice of the procedure for 99mTc discharge by high-selectivity methods (e.g., extraction, electrolysis, etc.), and also calls for optimization of the technology at all its stages. 2. PHYSICAL PRINCIPLES OF THE PROCESS 2.1. Paper [2] has described the results of computer simulation of 99Mo generation processes in liquid targets based on alkaline solutions of natural Mo. The advan- tages of these targets are the minimum number of proce- dures involving the solution, and also the ease of orga- nizing a loop-type cycle with target transportation be- tween the accelerator and the setup for 99mTc extraction. The disadvantages of the above targets lie in a low vol- ume activity of 99Mo (as a result of which it is advisable to realize this variant with the solution of isotopically pure 100Mo as a basis), and also in instability of saturat- ed solution as regards precipitation. The analysis of the data obtained shows that the highest yield of 99Mo in a solid natural molybdenum tar- get, 14.4 g in mass, makes 5 Ci per day for the 40 MeV beam of 10 kW power at a thickness of W converter of 1 mm and a thickness of converter-cooling water layer of 3 mm (this being in agreement with the results of ref. [3]). However, at these conditions a power of 3 kW is released in the target, and this makes the target cooling problematic. Here, as far as cooling is concerned, the operating conditions with a cylindrical beam of 30 MeV energy and up to 10 mm in diameter, appear real. In this case, the production of 99Mo is reduced down to 2.75 Ci per day, this however remaining acceptable as regards both general and specific activity of the target. 2.2. The main task of the undertaken experimental study of 99Mo generation processes at the electron accel- erator was to determine the yield of this isotope per unit charge of the beam as a function of accelerated electron energy for targets of different geometry and phase com- position. The targets were irradiated at the accelerators EPOS and KUT-20 [4]. 2.2.1. For experimental studies into the regularities of 99Mo production in water solutions a prototype of the target device has been developed [5]. It consists of a flowing water-cooled converter of bremsstrahlung and four cylindrical vessels axially symmetric to the elec- tron beam. The vessels were filled with a water solution of Na2MoO4 with a Mo concentration of 142 mg/ml. The experiments were performed at the EPOS accelera- tor at dose accumulation conditions for different elec- tron energies E0. Table 1 lists the measured volume activity values for the basic isotopes produced in 1 hour at an average beam current of 10 µA for each mode of irradiation. Table 1. Volume activity (A) of isotopes in target vessels (Na2MoO4) Е0, MeV № vess A, nCi/ml 90Mo 96Nb 99Mo 22Na 24Na 24 1 1.58 6.67 156.12 2.46 44.05 2 3.52 11.78 183.59 3.32 9.71 3 1.60 5.23 77.30 2.11 1.57 4 0.75 2.45 30.42 1.94 0.86 28 1 8.84 30.96 264.43 3.19 88.12 2 20.47 46.76 371.45 4.87 23.44 3 9.58 17.66 141.35 1.23 3.07 4 4.59 6.84 57.49 0.29 1.51 34 1 48.72 52.52 452.56 4.44 106.66 2 76.16 54.72 404.72 6.74 18.61 3 38.36 30.49 173.37 3.68 5.54 4 16.13 13.85 62.61 1.45 3.11 The reactions occurring only in the photonuclear channel can be used to separate the contributions of dif- ferent channels to the 99Mo generation. So, for the Na2- MoO4 solution these are 23Na(γ,n)22Na (Q= 4.12− MeV) ___________________________________________________________ PROBLEMS OF ATOMIC SIENCE AND TECHNOLOGY. 2004. № 1. Series: Nuclear Physics Investigations (42), p.168-171.168 and 92Mo (γ,2n)90Mo (Q=-13.1 MeV). The yield via the (n,γ) channel can be investigated with the 23Na(n,γ)24Na reaction. The data obtained with the help of the mentioned reactions on relative yields of 99Mo in (γ,n) and (n,γ) channels - Cγ and Cn (Cγ + Cn=1) are given in the report [5]. The analysis of the resulting data has shown that the solution of Mo, based on KOH, may appear more promising as a liquid target. This solution provides a higher concentration in Mo, gives less active wastes un- der irradiation, and also permits later on practically a di- rect separation of 99mTc by the extraction method. 2.2.2. Relying on the results of computer analysis, a target device (Fig.1) was designed to investigate the production of 99Mo in the solid phase. The device is arranged immediately behind the flow- ing water-cooled exit window (EW) of the accelerator. Inside the casing S there are a converter C (4 tantalum plates, each being 1 mm thick) and a target itself T in the form of a truncated cone which is axially symmetric to the electron beam. Н2О Н2О Т toe- EW S MoO3 Mo T2T1C Fig. 1. Device for investigating 99Mo generation in solid targets Two versions of the target were made: one (T1) - from metallic natural molybdenum, 30 g in mass; the other (T2) - as an aluminum capsule which encloses two foils from Mo and the MoO3 oxide, 50 g in mass. So, the two targets had nearly the same content of natural Mo. A thermocouple was placed inside each target to measure the temperature during irradiation. In these versions, the target was irradiated for 30 minutes at the accelerator KUT-20 at an electron energy of 30 MeV, an average current of 7 µA. Then, the total and specific activities of target elements were measured with the help of the Ge(Li) detector (see Table 2). In the process of irradiation, the steady-state temperature value at the center of the MoO3 target made up 75°C at a cool- ing water temperature of 36°C. Table 2. Activity of solid-target elements Target element Т1 Т2 Мо foil (front) МоО3 Мо foil (back) Acti- vity, МBq 8.249 0.142 5.70 0.065 3. BASIC SYSTEMS AND TREATMENT PROCEDURES The general scheme of the proposed 99Mo/99mTc pro- duction technology is presented in Fig.2. It is designed to accommodate the equipment within a single radia- tion-protection zone. The radioactive elements of the production cycle (target, irradiated structures, wastes, etc.) remain within the zone, and only the final product is removed from it in the form of sodium pertechnetate - 99mTc solution put into compact shipping containers and having the permissible level of radiation. The undertaken investigations have permitted us to formulate a set of requirements to be met by the basic systems of 99mTc production at the electron linac. The accelerator has electron energy up to 40 MeV, beam power no less than 10 kW, minimum transverse dimensions of the beam (<10 mm) and its angular diver- gence. The exit window of the accelerator at conditions of direct (unscanned) beam must have an operating life more than 1000 hours. The accelerator monitoring system must provide a continuous unperturbing monitoring of electron energy (average value), beam current (pulsed value and average value), and also of beam position within the exit win- dow. The target setup is designed in relation to the chosen version of the target (liquid, metallic Mo or MoO3). In any case, the cooling system of the complex must pro- vide the removal of heat power from the bremsstrahlung converter (no less than 3 kW) and from the target (no less than 0.5 kW). Therefore, it is advisable to make the converter rotating. The radiation durability of the setup structures must be no less than 1⋅1010 Gy. The sampling system is also determined by the cho- sen variant of the target. In all cases, it is reasonable to perform sampling and testing of the target at the initial stage of its irradiation. This is determined by the neces- sity of measuring the rate of generation of the main iso- topic product (99Mo) and by-products (for correcting, if necessary, the conditions of target processing), and by the possibility of safe handling the target. In the liquid target case, the sampling procedure consists in taking a 1...2 ml sample of irradiated solution with an activity up to 1 µCi. For the metallic Mo or MoO3 target, a sample, i.e., Mo foil, is placed at the exit of the target device, coaxi- ally with the target. The accelerator is switched on to be operated in the mode of target treatment, and the sample is activated up to ≤1 µCi. Then, the sample is forwarded to the gamma-spectrometer. To optimize the target irra- diation conditions and target adjustment with respect to the flow of braking photons, the method of measuring the surface activity distribution of the foil by means of a collimated CdZnTe radiometer has appeared to be rather efficient. The irradiated target transport system provides a re- mote discharge of the target (the equivalent dose rate (EDR) on the surface makes > 10 Sv/h) into a container, transportation of the container to the radiochemical lab- oratory, a remote-controlled withdrawal of the target and its transfer into the shielding box for further treat- ment. The system of target processing is determined by the form of the target. In the realistic version of the target based on natural molybdenum with a comparatively low activity (up to 3 Ci), the efficient separation of 99mTc is provided by the method of multiple extraction of 100Mo containing water solution by one and the same extrac- ___________________________________________________________ PROBLEMS OF ATOMIC SIENCE AND TECHNOLOGY. 2004. № 1. Series: Nuclear Physics Investigations (42), p.168-171.169 tant (methyl ethyl ketone) volume [6]. The final product is the solution of sodium pertechnetate-99mTc of standard activity, which is packed into flasks and undergoes ster- ilization. If the isotopically enriched 100MoO3 target is used, the radiochemical facility can readily be supplemented with a circuit for reduction of trioxide from the solution at the end of the 5-day cycle of 99mTc extraction for the repeat production of 99Mo at an accelerator. The isotope product quality control system involves a set of measuring devices and methods for determining the correspondence of the product to the Pharmacopoeia Regulations (PhR). The radioactive wastes (RAW) handling system pro- vides a stock-piling of wastes in temporary storages, and also a periodic control of RAW activity. The final-product transportation system includes portable shipping containers, which accommodate flasks with the solution of sodium pertechnetate-99mTc, and also specially equipped transport means for the delivery of containers to clinics. The radiation dosimetry system embraces all techno- logical procedures accompanied by the action of radia- tion on personnel. The requirements on the system and admissible levels of exposure are described in Radiation Safety Standards. 4. CONCLUSION The undertaken investigations have resulted in the elaboration of the fundamentals of a soft technology of 99mTc production for nuclear medicine with the use of the electron accelerator. The proposed process is fully compatible with the technologies in service today, based on the 98Mo(n,γ)99Mo reaction [6,7], as regards the pro- cedures of radiochemical extraction of 99mTc, prepara- tion of the solution of sodium pertechnetate-99mTc, pack- ing and sterilization, control of product quality and de- livery to the customers. These circumstances facilitate the procedure of new technology certification. R a d i a t i o n d o s i m e t r y Monitoring of electron beam parameters on the target Monitoring of target parameters during irradiation Monitoring of isotope product generation conditions Production of 99mТс: extraction, packing and sterilisation of products Sampling system Target recovery Monitoring of products to comply with the PhR Monitoring of quantity and activity of wastes Radioactive wastes handling system Electron accelerator Target complex Transport system Target processing system Product quality control system System of product shipping to the customer Fig.2. Functional block diagram of 99mTc production at the electron accelerator The use of the target enriched in the 100Mo isotope appears most efficient, both economically and ecologi- cally. For example, in the case of >95% enrichment, the yield of 99Mo increases by order of magnitude as com- pared with the target of natural composition. The activi- ty of liquid RAW produced in one technological cycle is reduced to the same extent. Though 100Mo is expensive (up to $5000 for 1 gram), a single purchase of 30 grams of the isotope provides a long-standing production of 99mTc. Really, in one cycle of irradiation, no more than 10-6 nuclei of 100Mo transmute into 99Mo, and after ex- traction of 99mTc, 100MoO3 can be easily reduced from the water phase to be used for the repeat irradiation. The use of reactor Mo accumulated in the wastes from spent fuel processing [8] is less expensive. The concentration of 100Mo in this case is 28% (9.6% in the natural Mo), i.e., the efficiency of the process is 3 times increased. 5. ACKNOWLEDGEMENTS The authors express their gratitude to L.V. Yeran for computer simulation of the processes of 99Mo genera- tion, to V.A. Shevchenko for the help in preparing and performing experiments, and to Yu.V. Lyashko for the gamma-spectrometric analysis of samples. The work has been supported by the STCU under Contract # 2185. REFERENCES 1. Isotopes for Medicine and Life Sciences. Editors S.G. Adelsten and F.G. Wanning. // Nat. Acad. Press, Washington, D.C. 1995, p.1, 4, 36, 40. 2. N.P. Dikiy, A.N. Dovbnya, S.V. Maryokhin, V.L. Uvarov. On Efficiency of Medical & Biophys- ical Isotopes Production Using Electron Accelerator // Problems of Atomic Science and Technology. Series: “Nuclear Physics Investigations” (34). 1999, № 3, р. 91-92. 3. R.G. Bennett et al. A System of 99mTc Production Based on Distributed Electron Accelerators and Thermal Separation // Nuclear Technology. 1999, p.102-121. 4. K.I. Antipov, M.I. Aizatsky, Yu.I. Akchurin et al. Electron Linacs in NSC KIPT: R&D and Applica- tion // Problems of Atomic Science and Technology. Series: “Nuclear Physics Investigations”. 2001, №1, p. 40-47. 5. N.P. Dikiy, A.N. Dovbnya, V.L. Uvarov. Electron Accelerator-Based Soft Technology for Medical Imaging Isotopes Production // Proc. of the 8-th European Particle Conference EPAC 2002 (Paris, 3-7 June 2002), p. 2760-2762. 170 6. A.I. Komov, V.S. Skuridin, A.G. Rybasov, V.M. Golovkov. New Technologies for Pharma- ceuticals on the Basis of Short-Lived Radionuclides Production // Izv. Vys. Ucheb. Zaved. 1998, N 4, p. 183-186 (in Russian) 7. A.V. Yegorov, M.P. Zykov, G.V. Korpusov et al. Production of 99mTc on the Centralized Generator in St. Petersburg // J.Nucl. Biol. Med. 1994, v. 38, № 3, p. 399-402. 8. S.A. Bartenev, M.P. Zykov, V.N. Romanovsky et al. Production of Molybdenum-99 & Technetium- 99m from Molybdenum-100 // Abstr. of 9-th Na- tional Conf. of Application of Charged Particle Ac- celerators in Medicine and Industry (22-24 Sept., 1998, St.-Petersburg, Russian), p.112 (in Russian). ОСНОВЫ ТЕХНОЛОГИЧЕСКОГО ЦИКЛА ПО ПРОИЗВОДСТВУ 99mТс НА УСКОРИТЕЛЕ ЭЛЕКТРОНОВ Н.П. Дикий, А.Н. Довбня, В.Л. Уваров Изложены результаты разработки физических и технологических основ производства 99Мо/99mТс с ис- пользованием тормозного излучения ускорителя электронов. ОСНОВИ ТЕХНОЛОГІЧНОГО ЦИКЛУ ПО ВИРОБНИЦТВУ 99mТс НА ПРИСКОРЮВАЧІ ЕЛЕКТРОНІВ М.П. Дикий, А.М. Довбня, В.Л. Уваров Викладені результати розробки фізичних і технологічних основ виробництва 99Мо/99mТс із використанням гальмівного випромінювання прискорювача електронів. ___________________________________________________________ PROBLEMS OF ATOMIC SIENCE AND TECHNOLOGY. 2004. № 1. Series: Nuclear Physics Investigations (42), p.168-171.171 N.P. Dikiy, A.N. Dovbnya, V.L. Uvarov National Science Center “Kharkov Institute of Physics and Technology”, 61108, Kharkov, Ukraine; E-mail: uvarov@kipt.kharkov.ua 1. INTRODUCTION REFERENCES
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last_indexed 2025-12-01T03:58:19Z
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spelling Dikiy, N.P.
Dovbnya, A.N.
Uvarov, V.L.
2015-03-25T19:26:33Z
2015-03-25T19:26:33Z
2004
The fundamentals of 99mTc production cycle at electron accelerator / N.P. Dikiy, A.N. Dovbnya, V.L. Uvarov // Вопросы атомной науки и техники. — 2004. — № 1. — С. 168-171. — Бібліогр.: 8 назв. — англ.
1562-6016
PACS: 06.60.Mr, 07.85.-m, 07.88+y, 81.30.Hd, 81.70.Jb
https://nasplib.isofts.kiev.ua/handle/123456789/79063
The report presents the results of investigations into physical and technological fundamentals of 99Mo/99mTc production with the use of bremsstrahlung of the electron accelerator.
Викладені результати розробки фізичних і технологічних основ виробництва 99Мо/99mТс із використанням гальмівного випромінювання прискорювача електронів.
Изложены результаты разработки физических и технологических основ производства 99Мо/99mТс с ис- пользованием тормозного излучения ускорителя электронов.
The authors express their gratitude to L.V. Yeran for computer simulation of the processes of 99Mo generation, to V.A. Shevchenko for the help in preparing and performing experiments, and to Yu.V. Lyashko for the gamma-spectrometric analysis of samples. The work has been supported by the STCU under Contract # 2185.
en
Національний науковий центр «Харківський фізико-технічний інститут» НАН України
Вопросы атомной науки и техники
Применение ускоренных пучков
The fundamentals of 99mTc production cycle at electron accelerator
Основи технологічного циклу по виробництву 99mТс на прискорювачі електронів
Основы технологического цикла по производству 99mТс на ускорителе электронов
Article
published earlier
spellingShingle The fundamentals of 99mTc production cycle at electron accelerator
Dikiy, N.P.
Dovbnya, A.N.
Uvarov, V.L.
Применение ускоренных пучков
title The fundamentals of 99mTc production cycle at electron accelerator
title_alt Основи технологічного циклу по виробництву 99mТс на прискорювачі електронів
Основы технологического цикла по производству 99mТс на ускорителе электронов
title_full The fundamentals of 99mTc production cycle at electron accelerator
title_fullStr The fundamentals of 99mTc production cycle at electron accelerator
title_full_unstemmed The fundamentals of 99mTc production cycle at electron accelerator
title_short The fundamentals of 99mTc production cycle at electron accelerator
title_sort fundamentals of 99mtc production cycle at electron accelerator
topic Применение ускоренных пучков
topic_facet Применение ускоренных пучков
url https://nasplib.isofts.kiev.ua/handle/123456789/79063
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