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Standardized High Current Solid Targets for Cyclotron Production of Diagnostic and Therapeutic Radionuclides

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Standardized High Current Solid Targets for Cyclotron Production of Diagnostic and Therapeutic Radionuclides TECHNICAL REPORTS SERIES No. 432 COMPANION CD-ROM STANDARDIZED HIGH CURRENT SOLID TARGETS FOR CYCLOTRON PRODUCTION OF DIAGNOSTIC AND THERAPEUTIC RADIONUCLIDES UNEDITED REPORTS OF THE PARTICIPANTS OF THE THIRD RESEARCH COORDINATION MEETING INTERNATIONAL ATOMIC ENERGY AGENCY VIENNA, 2004 CONTENTS Development of a high current solid target, a novel radiochemistry for Tl-201 and Pd-103 production R. Strangis, C. Rocco, E. Guevara, G. Maslat, F. Corral, N. Gonzáles, R. Téramo, J. Lago, G. Casale A plating/electrodissolution/recovery cycle for rhodium target material used for the industrial cyclotron production of palladium-103 P. van den Winkel, L. de Vis, R. Waegeneer, A. de Schrijver, H. Afarideh, M. Sadeghi, M. Haji Saeid New technology for the industrial preparation of high quality Tl-203 cyclotron targets by constant current electroplating P. van den Winkel, L. de Vis, M. de Vreese, R. Wageneer, A. de Schrijver, A. Arzumanov, N. Gorodiskaya, P. Zheltov Cyclotron production of iodine-123 and Pd-103 Zhou Wei, Wang Yongxian, Zhang Chunfu Production of diagnostic and therapeutic radionuclides S. Takács High current Tl-203, Rh-103 targets preparation for cyclotron production of Tl-201 and Pd-103 radionuclides A. Arzumanov, V. Berger, A. Borissenko, N. Gorodisskaya, I. Ilmatov, A. Knyazev, V. Koptev, S. Lyssukhin, A. Platov, G. Sychikov, D. Zheltov Research and technological development for the production of Pd-103 at the U-120 cyclotron from Bucharest P.M. Racolta, D. Dudu An operated solid target device design for iodine-123(124) production L.M. Solin, V.A. Jakovlev, A.I. Baranov, A.A. Timofeev, D.A. Zubov Standardized high solid targets for cyclotron production of diagnostic and therapeutic radionuclides S. Al Jammaz, S. Al-Yanbawi, S. Melibari, Rahma Useful concepts in solid state target technologies D.J. Schlyer, R.A. Ferrieri DEVELOPMENT OF A HIGH CURRENT SOLID TARGET, A NOVEL RADIOCHEMISTRY FOR TL-201 AND PD-103 PRODUCTION R. STRANGIS, C. ROCCO, E. GUEVARA, G. MASLAT, F. CORRAL, N. GONZÁLES, R. TÉRAMO, J. LAGO, G. CASALE Cyclotron Facility, Ezeiza Atomic Centre, Comisión Nacional de Energía Atómica, Argentina Abstract 201 P Solid targets development aims to obtain large quantities of radionuclides from accelerators.P Tl is the most used radioisotope in nuclear medicine, which is produced in cyclotron. The scope of the research was to test another procedure of Tl-201 production as an alternative of the precipitation and extraction method used at present. Utilization of ionic exchange resins was studied. Pd-103 is increasingly used in brachytheraphy seeds. A high current solid target technique for cyclotron irradiation of electroplated metals was developed to produce Tl-201 and Pd-103. The design of the solid target set up and different procedures to obtain Pd-103 for seeds applications are presented. 1. INTRODUCTION Tl-201 has wide utilization in cardiologic studies, renal, and in the last years as tumoural 103 P cerebral detector. P Pd has been used in treatment of various cancers such as eye, brain, neck, uterus, colon [1], but it is almost exclusively used for prostate cancer as the most common cancer and causing the highest death rate in men. These radionuclides are cyclotron-produced by irradiation of solid targets and the objective of this CRP is to develop procedures to obtain these targets. 2. DEVELOPMENT OF A NEW SOLID TARGET CARRIER The solid target system installed in the Cyclotron Facility by Forschungszentrum Karlsruhe o P (FZK), Germany, has the following characteristics: Tangent beam 7P , ISO-RABBIT pneumatic transport system; welded system, Al body + Ag face, Irradiation surface of 23 mm × 80 mm. 203 P Problems after 160 P Tl irradiations: • High cost: US$1800 • Recovery needed: High dose (Ag-105) 6 month of decay to reuse. • 30 Targets for a weekly routine production + • P AgP ions are introduced with Tl-203. Pitting of the silver surface reduce the life. • Cooling studies made by Prof. Van Den Winkel show that at 100 µA metallic thallium melts. • Ag+ traces are recovered with enriched Tl (same cationic group) The proposed target has the following advantages: • Screwed system, no weld needed. • Frontal face: 1mm Cu (not recycled) thickness • Two-pieces target. Al body (low dose, recycled) Cu face, (high dose, not recycled). • Low assembly dose. • 3-4 target body/weekly irradiation. • Low irradiation cost. 103 • P Allows Rh irradiation for P Pd production; better cooling. 1 FIG. 1. Ezeiza target. TABLE I. DEFORMATION OF DIFFERENT CU SHEETS (MM) Thickness Pressure 2 2 2 P P P 1 Kg/cmP 3 Kg/cmP 7 Kg/cmP 1 mm - 0.02 0.04 1.5 mm - 0.01 0.02 2 mm - - 0.01 3. NEW CHROMATOGRAPHIC TL/PB SEPARATION FOR TL-201 CYCLOTRON PRODUCTION 3.1. Analytical methods + 3+ 2+ P P P The distribution constants (Kd) of TlP , TlP and PbP were determined for the cation exchange resin BioRad AG-50W of different cross-linkages and particle sizes and different HCl and HNO3B B 201 2+ 210 P P P concentrations. To measure Tl tracer of P Tl, was used to detect PbP tracer of P Pb was involved. The concentrations of Tl measured in the Jarrell-Ash equipment by atomic emission (sensibility 1.0 ppm) at 3445 Å were correlated with Pb measured in the same equipment at 2170 Å (sensibility 0/01ppm). 2 The chromatographic separation was developed using preparative equipment constituted by a peristaltic pump, a GILSON fractions collector coupled to a NaI (Tl) detector and a home made data acquisition system. 3.2. Determination of Kd 1,000 g of cationic resin in 50 ml acid solution was equilibrated with 250 mg of Tl2B SO4B labeled 201 2+ 210 P P P with P Tl. For the PbP , a solution of Pb (NO3B )B 2B B (concentration 0.1mg/ml) spiked with P Pb was used. 201 3+ 201 + P P P P The P TlP was obtained oxidizing the P TlP with a Cl 2B B generator (KMnO4B B + HCl) bubbling gently during one minute and then heating in order to eliminate the residual Cl2B .B Table II shows the Kd values obtained with AG50Wx12, 200-400 mesh resin for different concentration of HCl and HNO2.B TABLE II. KD RESULTS [HNO3B ]B 0.1 M 0.25 M 0.5 M 1.0 M 2.0 M 5.0 M 2+ 4 P P PbP 10P 1420 183 35 8.5 7.2 + P TlP 173 91 41 22.3 9.9 7.6 [HCl] 0.1M 0.25 M + P TLP 100 62 3+ P TlP 80 53 2+ 4 P P PbP 10P 3500 3.3. Optimization of the chromatographic Pb/Tl separation 201 210 P P Using a simulated target (700 mg of TlNO3B B and 1mg of Pb (NO)2B B labeled with P Tl and P Pb respectively) in a low pressure chromatographic equipment, separations involving different types of columns, resin bulks, gradients and solvent flows were tried. The optimal conditions for the separation are, as follows: • Type of Resin: AG50WX12 200-400 • Solvent: HNO3B B 0.1M • Resin bulk: 1,20 g • Flow: 1.3 ml / min • Temperature: ambient + + 2+ P P P In these conditions, a high ratio of Kd PbP /TlP in HNO3B B 0.1M is found, allowing to keep PbP + P adsorbed on the column during quantitative elution of Tl P . 3.4. Proposed method The previous results allow to realize a new separation of 203Tl carrier from the carrier-free 201Pb after dissolution of the irradiated target in diluted HNO3 and adsorption on a small AG-50W X12 203 P (200-400 merk) column. The P Tl is quantitatively eluted with 0,1 MHNO3 and 0,1 MHCl. Upon a 32 hrs decay period, the 201Tl is eluted with 0,1 MHCl. The flow diagram is represented in Fig. 3. 3 HNO .1M HCL .1M HCL 2M 150 Tl Pb 100 50 0 0 50 100 150 200 250 300 350 400 450 FIG. 2. Chromatogrammes. 201 201 P P FIG. 3. Method of cyclotron produced P Tl using chromatographic withholding in P Pb column. The solution obtained in the 203Tl recovery step is HNO3 0.1M, a medium allowing use as such in the recovery step of 203Tl. The active residues from Pb obtained in the last step were used to study the percentage of Pb2+, remaining on the column and by the isotopic relationship, the energy range to which was irradiated the target. 3.5. Target irradiation 203 201 201 P P P P The main production reaction is: P Tl (p, 3n) P Pb Tl (t½=73hs) 4 and the secondary reactions are: 203 203 P P P Tl (p, n) P Pb (t½=52hs. ) 203 202 202 P P P P P Tl(p,2n)P Pb Tl(t½=12.2 d) 203 200 200 P P P P P Tl (p, 4n) P Pb Tl(t½ = 26.1hs) From the ALICE code and according to literature (8, 9) it follows that the optimum irradiation + P range with HP is 28 to 18Mev. This range minimizes the impurities produced by the secondary reactions, in order to produce a final product according the pharmacopoeia regulations. A target thickness corresponding with such energy degradation was produced and sufficient surface area for the power dissipation of the cyclotron beam (3 kw) was realized. o P For solid targets, the proton beam target angle equals 7P . The target area consists of an ellipse 203 P (to 7 degree projection of a circle of 10 mm in diameter) of 80 * 10 mm with 700 mg of P Tl (98%), electroplated in basic medium according Van den Winkel’s recommendations in a double window cube.
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