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Production of medical radioisotopes 68Ga and 45Ti in deuteron-induced reactions in cyclotrons

Tsoodol, ZOLBADRAL 北海道大学

2021.09.24

概要

Positron Emission Tomography (PET) is a powerful nuclear imaging technique based on an annihilation reaction of a positron and an electron. A positron emitted from a radiopharmaceutical injected into a patient reacts with an electron in tissue and decays into two 511-keV gamma rays. The positron emitter contained in the radiopharmaceutical is essential for the imaging technique. A variety of positron emitters can be used, and their production is worth investigation.

The dominant method to produce the positron emitters is charged-particles-induced reactions in cyclotrons. Generators and neutron-induced reactions can also produce a few positron emitters. Although most PET isotope production routes are well established, there is still a need for continuous research and development for better route and more efficient radionuclides. Nuclear reaction data are required for such research and development. Based on the nuclear reaction data, we can select projectile and targets and optimize the projectile energy to maximize the yield of the desired product and to minimize co-produced impurities.

Positron emitters 68Ga and 45Ti are expected to become more popular in clinical PET scanners. Their promising production routes can be considered as the (p,n) reactions on isotopically enriched targets of 68Zn and 45Sc. Alternative production routes are the (d,2n) reactions on 68Zn and 45Sc. In the literature, a few experimental cross section data on deuteron-induced reactions for production of 68Ga and 45Ti were reported. In addition, there are significant discrepancies among them. Therefore, we aimed to investigate the deuteron- induced reactions to produce 68Ga and 45Ti to investigate the production routes.

The production cross sections of deuteron-induced reactions on natural zinc for 68Ga and on scandium for 45Ti were measured up to 24 MeV, respectively. The measured excitation functions were compared with previous experimental data and the theoretical model calculation of the TENDL library. The physical yields for 68Ga and 45Ti production were deduced from the measured cross sections and compared with previous experimental data.

Two experiments were carried out to measure reliable data on the production cross sections of 68Ga and 45Ti in deuteron-induced reactions on natural zinc and scandium. The two experiments were performed at the AVF cyclotron of RIKEN RI Beam Factory. Stacked-foil activation technique and γ-ray spectrometry were used to measure the cross sections. Two stacked targets were prepared and irradiated with deuteron beams. The incident beam energies were measured by the time-of-flight method. The energy degradation in the stacked foils was calculated using the SRIM code. The beam intensities were measured by Faraday cups and cross-checked using the natTi(d,x)48V monitor reaction. γ-ray spectra of the irradiated foils were measured by high- resolution HPGe detectors without chemical separation. The detectors were calibrated by a standard mixed multiple γ-ray emitting point source.

For the 68Ga experiment, the stacked target was composed of metallic foils of natZn (17.64 mg/cm2, 99.9% purity) and natTi (9.13 mg/cm2, 99.6% purity). The target was irradiated for 22 min by a 24-MeV deuteron. The measured beam intensity was corrected to 102.4 nA by increasing 6.6% from the measured value according to comparison of the monitor reaction. The distance between the detector and the foils was chosen to keep the dead time less than 7%.

The excitation functions of the natZn(d,x)68Ga reaction were measured up to 24 MeV. Production cross sections of co-produced radioisotopes 65,66,67Ga, 63,65,69mZn, 61Cu and 58Co were also determined. The derived excitation function of the natZn(d,x)68Ga reaction is consistent with the data of Šimečková et al. (2017). The deduced physical yield of 68Ga partially agrees with the previous data. The yields of proton- and deuteron- induced reactions on 68Zn for 68Ga production are compared. The yield of the 68Zn(d,2n)68Ga reaction is found to be comparable with that of the 68Zn(p,n)68Ga reaction. The data obtained in this work are useful to consider the best reaction to produce 68Ga for practical use.

For the 45Ti experiment, the stacked target consisted of metallic foils of 45Sc (7.71 mg/cm2 thickness, 99.0% purity and 76.0 mg/cm2 thickness, 99.0% purity), 27Al (4.99 mg/cm2, 99.6%) and natTi (9.13 mg/cm2, 99.6%). The target was irradiated for 30 min with a 24-MeV deuteron beam. Based on comparison of the monitor reaction, the intensity was corrected to 175.2 nA by decreasing 3% from the measured value (180.3 nA). The dead time was kept below 7% in the measurements.

The excitation functions for the production of 45Ti and co-produced radioisotopes such as 44Ti and 44g44m,46Sc was measured up to 24 MeV. The derived excitation function of the 45Sc(d,2n)45Ti reaction is consistent with the earlier published data of Hermanne et al. (2012). The deduced physical yield of 45Ti is slightly larger than the previous experimental data. The radioactive-contamination-free 45Ti can be obtained via the 45Sc(d,2n)45Ti reaction in the energy region of 15 - 8 MeV applying chemical separation.

In conclusion, we investigated the deuteron-induced reactions on natural zinc and scandium. The production cross sections of 68Ga and 45Ti were determined. Based on the results, the deuteron-induced reactions on enriched 68Zn and natural scandium can be alternative routes for cyclotron production. The data measured in these experiments extend the nuclear reaction database and are available for optimizing production routes of the medical isotopes.

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