Production of Sc medical radioisotopes with proton and deuteron beams.

Proton and deuteron beams (15.3 and 6.8 MeV, respectively) extracted from the PETtrace medical cyclotron at the Radiopharmaceuticals Production and Research Centre in the University of Warsaw, Heavy Ion Laboratory, 28 MeV protons from the C30 cyclotron at the National Centre for Nuclear Research, Swierk, near Warsaw and 33 MeV protons from the ARRONAX accelerator, Nantes were used to produce and investigate the medically interesting Sc radioisotopes. Both natural and isotopically enriched CaCO3 and TiO2 targets were used (42Ca, 43Ca, 44Ca, 48Ca, 48Ti). The production efficiency and isotopic purity were determined and are reported here for the highest commercially available enrichments of the target material. The Thick Target Yield, Activities at the End of Bombardment (EOB) and the relative activities of produced impurities at EOB are reported for 43Sc, 44gSc, 44mSc and 47Sc produced with particle energies below 33 MeV.

Production of medical Sc radioisotopes with an alpha particle beam.

The internal α-particle beam of the Warsaw Heavy Ion Cyclotron was used to produce research quantities of the medically interesting Sc radioisotopes from natural Ca and K and isotopically enriched 42Ca targets. The targets were made of metallic calcium, calcium carbonate and potassium chloride. New data on the production yields and impurities generated during the target irradiations are presented for the positron emitters 43Sc, 44gSc and 44mSc. The different paths for the production of the long lived 44mSc/44gSc in vivo generator, proposed by the ARRONAX team, using proton and deuteron beams as well as alpha-particle beams are discussed. Due to the larger angular momentum transfer in the formation of the compound nucleus in the case of the alpha particle induced reactions, the isomeric ratio of 44mSc/44gSc at a bombarding energy of 29MeV is five times larger than previously determined for a deuteron beam and twenty times larger than for proton induced reactions on enriched CaCO3 targets. Therefore, formation of this generator via the alpha-particle route seems a very attractive way to form these isotopes. The experimental data presented here are compared with theoretical predictions made using the EMPIRE evaporation code. Reasonable agreement is generally observed.

Cyclotron production of (43)Sc for PET imaging.

BACKGROUND: Recently, significant interest in (44)Sc as a tracer for positron emission tomography (PET) imaging has been observed. Unfortunately, the co-emission by (44)Sc of high-energy γ rays (E γ = 1157, 1499 keV) causes a dangerous increase of the radiation dose to the patients and clinical staff. However, it is possible to produce another radionuclide of scandium-(43)Sc-having properties similar to (44)Sc but is characterized by much lower energy of the concurrent gamma emissions. This work presents the production route of (43)Sc by α irradiation of natural calcium, its separation and purification processes, and the labeling of [DOTA,Tyr3] octreotate (DOTATATE) bioconjugate. METHODS: Natural CaCO3 and enriched [(40)Ca]CaCO3 were irradiated with alpha particles for 1 h in an energy range of 14.8-30 MeV at a beam current of 0.5 or 0.25 µA. In order to find the optimum method for the separation of (43)Sc from irradiated calcium targets, three processes previously developed for (44)Sc were tested. Radiolabeling experiments were performed with DOTATATE radiobioconjugate, and the stability of the obtained (43)Sc-DOTATATE was tested in human serum. RESULTS: Studies of (nat)CaCO3 target irradiation by alpha particles show that the optimum alpha particle energies are in the range of 24-27 MeV, giving 102 MBq/µA/h of (43)Sc radioactivity which creates the opportunity to produce several GBq of (43)Sc. The separation experiments performed indicate that, as with (44)Sc, due to the simplicity of the operations and because of the chemical purity of the (43)Sc obtained, the best separation process is when UTEVA resin is used. The DOTATATE conjugate was labeled by the obtained (43)Sc with a yield >98 % at elevated temperature. CONCLUSIONS: Tens of GBq activities of (43)Sc of high radionuclidic purity can be obtainable for clinical applications by irradiation of natural calcium with an alpha beam.

Correlation between radioactivity induced inside the treatment room and the undesirable thermal/resonance neutron radiation produced by linac.

High-energy therapeutic beams used in the radiotherapy induce photonuclear and electronuclear reactions which are accompanied by generation of undesirable radioisotopes and neutrons inside the treatment room. These neutrons at thermal and resonance energies induce nuclear reactions through the whole accelerator bunker. In consequence various radioisotopes emitting high-energy photons appear. In this paper the correlation between radioactivity induced inside the treatment room and the undesirable thermal and resonance neutron radiation generated by the therapeutic accelerator X-rays was studied. The thermal and resonance neutron fluence determined in chosen places inside the bunkers was 1.0x10(5)-3.4x10(5)cm(-2)Gy(-1) and 1.0x10(5)-1.6x10(6)cm(-2)Gy(-1) at thermal energies (<0.1eV) and 3.9x10(4)-1.3x10(5)cm(-2)Gy(-1) and 1.0x10(5)-1.1x10(6)cm(-2)Gy(-1) at epithermal energies (0.1eV-10keV), for the 15MV and 20MV beams, respectively. The gamma energy spectra measured inside the accelerator bunker depended on the neutron radiation level. The net count rates of the gamma peaks from the decays of the excited state (56)Fe* and (28)Si*, the result of the simple capture of the neutron, for the 20MV beam were almost one order of magnitude greater than those for the 15MV beam. Moreover, it turned out that the activation of the wedge - the main accelerator accessory was caused by neutrons.

Undesirable nuclear reactions and induced radioactivity as a result of the use of the high-energy therapeutic beams generated by medical linacs.

In this paper, the problem of undesirable photonuclear, electronuclear and neutron capture reactions taking place in the treatment room during emission of the typical high-energy therapeutic beams from two different medical accelerators, i.e. Primus Siemens and Varian Clinac-2300, is presented. The radioisotopes (187)W, (56)Mn, (28)Al, (57)Ni, (38)Cl, (57)Co and (19)Au and the neutron activation of (1)H were identified as a consequence of these reactions. Moreover, the increased photon fluence rate behind the door of the accelerator bunker in the operator console room was observed during emission of the 20 MV X-rays from the Varian Clinac-2300 as well as in the case of the 15 MV X-ray beam from the Primus Siemens. No increased radiation was observed during the 6 MV X-ray beam emission. The performed measurements produced evidences on the presence of neutrons in the operator console room during emission of the 15 MV X-ray beam from the Primus Siemens as well as the 20 MV X-rays and the 22 MeV electrons from the Varian Clinac-2300 accelerator.