Large-scale production of 88Y and 88Zr/88Y generators: A proof of concept study for a 70 MeV H- cyclotron.

The large-scale production of 88Y with proton-induced reactions has been investigated from the perspective of new generation 70 MeV H- cyclotrons. Tandem target configurations are presented for both the direct production of 88Y as well as for producing 88Zr/88Y generators. Based on the relevant excitation functions, physical yields have been derived for 88Y production with Y2O3/SrCO3 tandem targets and 88Zr production with Zr/Y2O3 tandem targets. Yields are presented for optimized targets (i.e. optimum yield) as well as for balanced thermal loads on the individual targets. Liquid 88Zr/88Y generators have been produced using both natural Zr and Nb target materials, the former for dedicated productions and the latter as a byproduct by processing spent irradiated Nb capsules which normally would constitute radioactive waste. These stock solutions, which contain both the target material and 88Zr precursor, are retained virtually unchanged after processing except for the removal of 88Y on AG MP-50 macroporous cation-exchange resin. Methods are presented for the preparation of Nb stock solutions in hydrofluoric acid and Zr stock solutions in sulphuric acid. It is shown that multi-Ci productions of 88Y are feasible at a 70 MeV cyclotron facility, suitable for the needs of fracking applications. In addition, 88Zr/88Y generators can provide 88Y with very high specific activity, suitable for labelling of biomolecules. LA-UR-20-24305.

Pairing of thorium with selected primary target materials in tandem configurations: Co-production of 225Ac/213Bi and 230U/226Th generators with a 70 MeV H- cyclotron.

Several radionuclide production facilities based on a new generation of high-current, 70 MeV H- cyclotrons have been established in recent years and a number of new facilities are either under construction or being planned. In this study, the feasibility to produce 225Ac/213Bi and 230U/226Th generators via Th + p reactions at such a facility has been investigated. From the perspective of production yields, it has been found useful to compare the relevant reactions on thorium with those on other targets regularly employed in this energy region, in particular the natMg(p,x)22Na, natGa(p,x)68Ge, and natRb(p,x)82Sr reactions that have been exploited with 66 MeV proton beams at iThemba LABS for many years. Therefore, various tandem configurations of thorium with magnesium, gallium and rubidium are discussed based on the relevant nuclear data. In a few cases, the available data were judged to be insufficient in this energy region. New experimental cross sections are presented for 225Ac, 225Ra, and 230Pa in Th + p reactions as well as 22,24Na in natMg + p reactions. Integral yields have been derived for those radionuclides of main interest. Production yields expected from extended 70 MeV proton bombardments, on selected tandem-target configurations, are presented for 22Na, 68Ge, 82Sr, 225Ac, and 230Pa. It is concluded that 225Ac/213Bi generators can, in principle, be added to a production programme based at a 70 MeV H- cyclotron facility as the production rate is of similar magnitude to those of other well-established radionuclides in this energy region. Also, radio-contaminant levels for 225Ac are similar to those found in higher proton-energy windows. The scope for 230U/226Th generators, via bulk production of the precursor 230Pa, seems to be more limited due to a lower yield but can nevertheless be produced in clinically relevant quantities.

Concurrent spectrometry of annihilation radiation and characteristic gamma-rays for activity assessment of selected positron emitters.

A method is described to determine the activity of non-pure positron emitters in a radionuclide production environment by assessing the 511keV annihilation radiation concurrently with selected γ-lines, using a single High-Purity Germanium (HPGe) detector. Liquid sources of 22Na, 52Fe, 52mMn, 61Cu, 64Cu, 65Zn, 66Ga, 68Ga, 82Rb, 88Y, 89Zr and 132Cs were prepared specifically for this study. Acrylic absorbers surrounding the sources ensured that the emitted ß+-particles could not escape and annihilate away from the source region. The absorber thickness was matched to the maximum ß+ energy for each radionuclide. The effect on the 511keV detection efficiency by the non-homogeneous distribution of annihilation sites inside the source and absorber materials was investigated by means of Monte Carlo simulations. It was found that no self-absorption corrections other than those implicit to the detector calibration procedure needed to be applied. The medically important radionuclide, 64Cu, is of particular interest as its strongest characteristic γ-ray has an intensity of less than 0.5%. In spite of the weakness of its emission intensity, the 1346keV γ-line is shown to be suitable for quantifying the 64Cu production yield after chemical separation from the target matrix has been performed.

Production cross sections of radioisotopes from 3He-particle induced nuclear reactions on natural titanium.

Excitation functions were measured using the stacked-foil method for the natTi(3He,x)44mSc, 46m+gSc, 47Sc, 48Sc, 48V and 48Cr nuclear processes up to 68MeV. Our new cross-section data were compared with the earlier reported values as well as the evaluated theoretical predictions by means of the TALYS 1.6 code as compiled in the TENDL-2015 library. The new data show acceptable agreement with the previous experimental values in the overlapping energy regions, however only a partial agreement was found in the case of the results of the nuclear reaction model code. The present work not only strengthens the experimental datasets of the above processes but also provides new cross-section values above 36MeV where only one dataset is available for each reaction.

The production of (88)Y in the proton bombardment of (nat)Sr: New excitation and separation studies.

The cyclotron production of (88)Y at iThemba LABS is performed via the reaction (88)Sr(p,n)(88)Y. The yields obtained were inconsistent with nuclear data obtained from the literature and the excitation function of the nuclear reaction was re-measured, using a differentiation of thick-target production rate measurements. Ion exchange chromatographic methods are described to separate (88)Y from (nat)Sr target material using AG MP-1 resin and AG 50W-X4 resins, respectively.

Excitation functions of 3He- and alpha-particle induced nuclear reactions on natSb for production of medically relevant 123I and 124I radioisotopes.

Excitation functions were measured using the stacked foil irradiation technique from threshold energies to 28 MeV for (3)He- and to 21 MeV for alpha-particle induced nuclear reactions on natural antimony leading to the formation of (121,123,124)I radioisotopes. The measured excitation functions were compared with the contradicting results of the earlier investigations found in the literature and with the curves predicted by the ALICE-IPPE and EMPIRE-II codes. Integral yields were also calculated and compared with the experimental thick target yields reported in the literature.

Comments on the feasibility of 61Cu production by proton irradiation of (nat)Zn on a medical cyclotron.

Feasibility of 61Cu production in high radionuclidic purity form via (nat)Zn(p,x) 61Cu nuclear process is discussed. Based on the experimentally available cross-sections of the (nat)Zn(p,x) 61Cu, (nat)Zn(p,x) 60Cu and (nat)Zn(p,x) 64Cu nuclear processes the usefulness of the (nat)Zn(p,x) 61Cu process for high-scale production is questionable in the 22 --> 12 MeV energy range.

Cross sections of proton induced nuclear reactions on enriched 111Cd and 112Cd for the production of 111In for use in nuclear medicine.

Proton induced nuclear reactions on enriched 111Cd and 112Cd have been studied up to 30 MeV in the context of routine production of the medically used isotope 111In with low and medium energy cyclotrons. The excitation functions of 111Cd(p,n)111m,gIn and 112Cd(p,2n)111m,gIn as production reactions and 111Cd(p,2n)110mIn, 111Cd(p,2n)110In, 111Cd(p,3n)109ml,m2,In, 112Cd(p,3n)110mIn, 112Cd(p,3n)110gIn as competing processes have been measured using the activation method involving the stacked-foil technique. The deduced thick target yields are compared with those obtained experimentally.

Temperature course in small volume [18O]water targets for [18F]F- production.

In order to understand the thermal processes occurring within a water target we carried out calculations of heat transfer of the beam energy absorbed from the target water to the target back wall, and compared them with the temperatures measured during irradiations. It was shown, by both the experimental results and the heat transfer calculations, that, at high beam currents, static small volume water targets have a working temperature at the boiling point of the target water. The heat transfer occurs only by movement of the water molecules generated by the boiling target water and not by heat conduction or free convection alone. There is no heat transfer arising from vaporization and reflux.