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Dosimety of FDG-18F Produced at the SOREQ Cyclotron CYCLONE 5/10

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Dosimety of FDG-18F Produced at the SOREQ Cyclotron CYCLONE 5/10 Production Yield of 18F-FDG at the SOREQ NRC Cyclotron CYCLONE 5/10 G. Haquin, M. B. Goldberg, Y. Ben Meir , T. Arbel and D. Ben Maman Soreq Nuclear Research Center, Yavne 81800, [email protected] Keywords: 18F-FDG, cyclotron, dose calibrator, PET. Abstract The SOREQ NRC proton cyclotron accelerator CYCLONE 5/10 began producing 18F- FDG at the beginning of 2001. 2-Fluoro-2 deoxy D-Glucose (FDG) labelled with radioactive 18F is used for Positron Emission Tomography (PET) imaging in medical diagnostic procedures. The FDG solution is produced at Soreq’s radiopharmacy following proton irradiation 18 18 of heavy water H2 O and chemical synthesis of the F-FDG compound at the cyclotron site. In the present work we have measured the absolute activity of 18F and FDG-18F produced and checked the accuracy of the dose calibrator measurement for 18F. The chemical reactor efficiency for synthetization of FDG was also determined. Introduction The Cyclone 5/10 supplies protons of 10 MeV nominal energy by accelerating hydrogen ions in a cyclotron. The beam is extracted to a Havar window of 25µm 18 18 thickness and bombards a H2 O water target. F is produced via the reaction 18O(p,n)18F, which has a peak in the cross section for proton energies between 5 and 8.5 MeV [1]. The reaction yield can be approximately expressed by the following expression: IA Y ≈ N p ⋅ σ TOT ⋅TTeff (1) Where Y is the reaction yield, Np is the number of protons (given by the beam ΙΑ current), <σΤΟΤ > is the average cross section for the reaction and TTeff is the effective target thickness. For a target containing 94% of 18O, 2% of 17O and 4% of 16O, the radionuclides produced are given in Table 1. The stated reaction yield corresponds to an irradiation at 80µA (4.8x1014 p/sec)). For 13N and 17F the activity is in saturation. In addition to the above positron-emitting radionuclides, the stable isotopes 15N, 18O, 19F and 16O are produced. IA Isotope Reaction <σtot > (mb) Yield T1/2 [min] 18F 18O(p,nγ)18F ~210 (n) 2.71 [1011/s] 109.8 17F 17O(p,nγ)17F ~2.5 (n) ~90mCi (sat) 1.075 17F 16O(p, γ)17F <4x10-4 <20µCi (sat) 1.075 13N 16O(p,α)13N ~1.5 ~30mCi (sat) 9.965 18 Table 1: Radioactive reaction products produced by proton bombardment of H2 O. The accuracy of these calculations is not expected to be better than 10%. Material and Methods 18 In the present study, three irradiations of an H2 O target (approximately 2.2 ml) containing 18O: 95.3%, 17O: 2.3% and 16O: 2.4% were performed. The first two irradiations investigated the output of the cyclotron and the third irradiation investigated the chemical reactor module for synthetization of 18F-FDG. The layout of the experiments is shown in figure 1. Experiment 3 18 Proton beam H2 O target cell Chemical synthetization of FDG-18F Experiment 3 Experiment 1 + 2 Dose calibrator Figure 1: Schematic layout of the experiments. The activity was measured using an absolutely-calibrated dose calibrator for nuclear medicine model CRC-35R (Capintec Inc.)[2]. The dose calibrator consists of a pressurized ionization chamber which converts the gamma-induced ion chamber current into activity. A dial setting of 439 is the manufacturer’s recommended value for 18F. The manufacturer dial setting is a theoretical value calculated by interpolating along the calibration curve. This value is somewhat geometry-dependent [3] and therefore, its accuracy was checked for a 5ml dose vial geometry measuring an aliquot of the master solution gravimetically dispensed into a container and measured by a calibrated high resolution gamma spectrometry based on a HPGe detector. The activity measured with the dose calibrator is a combination of the isotopes produced: 18F, 17F and 13N which are pure positron-emitters, therefore, the dial setting of the instrument remains the same for all of them. The differences in nuclide half life is exploited to determine the activity of each isotope, solving an exponential decay function of third order that has the following form: −(λ ⋅t) −(λ ⋅t) −(λ ⋅t) A(t) = A exp 18F + A exp 13F + A exp 13N (2) 18F 17F 13N −(λ ⋅t) for t >> τ ⇒ A(t) = A exp 18F 13N 18F The chemical reactor module synthetizes the 18F produced in the cyclotron into the FDG compound [4]. The chemical process takes approximately 25 minutes, in the course of which the isotopes of fluorine are separated from the irradiated solution and the 17F decays completely (more than 20 half lives). The resulting compound is 18F- FDG, the activity of which is lower than the yield produced at irradiation due to radioactive decay and the efficiency of the chemical process. Results Three experiments were performed under nominally identical irradiation conditions, in order to check reproducibility. The irradiation conditions of the large volume target (2.2ml) were: total proton current 3µA, irradiation time 27 minutes. For this irradiation time, the 17F is in saturation, which is not the case for 18F, nor for 13N. The isotope calibrator readout was monitored over two hours, yielding the graph displayed in figure 2. 100 ) Ci (m ty i tiv c a tal o T 0 20 40 60 80 100 120 Time (min) Fig. 2: Total activity measured with dose calibrator and exponential decay fit. The activity of the isotopes was derived from the data using eq. 2 and the results are detailed in Table 2. The calculated values correspond to a theoretical calculation based on tabulated cross sections, using eq. 1 [1]. In experiment 3 the programmed value represents the calculated activity, multiplied by the manufacturer-stated chemical efficiency of 65% (which includes the radioactive decay of 18F during 25 minutes of synthesis). Isotope Experiment 1 Experiment 2 Experiment 3 Activity (mCi) Activity (mCi) Activity (mCi) Calculated Measured Calculated Measured Programmed Measured 18 F 117 105±7 117 108±8 76.1 71.5±5.0 17F 10.9 11.7±1.8 10.9 9.3±1.4 13N 1.6 1.3±0.3 1.6 2.5±0.5 The stated uncertainties are at 2σ. Table 2: Activity measured and calculated for the three experiments. The activity of 13N was found to be within the uncertainty of the measurement of 18F. The calibration of the dose calibrator dial setting for 18F was performed using HPGe detector and its accuracy was found to be within 3.5%, which is within the acceptable tolerance for nuclear medicine purposes. Conclusions Dosimetry measurement of 18F-FDG produced at the SOREQ cyclone 5/10 were performed. Good agreement between measured and calculated values was found. The accuracy of the dial setting of the dose calibrator for 18F activity measurements at 10ml vial geometry was found to be within 3.5%. The chemical reactor efficiency was found to be 80% (68% including the radiactive decay of 18F). References: [1] M. Goldberg, D. Berkovits, A. Tal and Y. Shamai; “Expected Radiation Levels from Reactions of a 80µA, 10 Mev Proton Beam on a 18O Enriched Water Thick Target and Radiation Protection Resources”, Soreq report 2993, 1999, in Hebrew. [2] Capintec Inc,. “Radioisotope Dose Calibrator Owner’s Manual”, Rev E, Ramsey, NJ,1997. [3] B.E. Zimmerman and J.T. Cesna; “Experimental Determination Of Commercial ‘Dose Calibrator’ Settings For Nuclides Used In Nuclear Medicine”, Applied Radiation and Isotope, 52 (2000) 615-619. [4] Coincidence Technologies s.a., FDG Synthesizer User Manual, 2000. .
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