New method for production of 155Tb via 155Dy by irradiation of natGd by medium energy alpha particles

Abstract

Introduction: ¹⁵⁵Tb (T_1/2 = 5.32 d) is considered both as a promising Auger electron emitter and as a diagnostic pair for other therapeutic terbium radionuclides. Despite several methods for its production proposed, it remains scarcely available. Most of the methods using low-energy protons and deuterons beams result in a high content of radionuclidic impurities. High purity ¹⁵⁵Tb can be obtained using high-energy proton beams combined with online mass separation of products, but the method remains inaccessible to most potential consumers. We have proposed an indirect method for the production of ¹⁵⁵Tb via formation of ¹⁵⁵Dy (T_1/2 = 9.9 h), which can be implemented using medium energy alpha particles beam.

Methods: Gadolinium oxide targets of natural isotopic composition were irradiated by 60 MeV alpha particles beam on a U-150 cyclotron of the National Research Center "Kurchatov Institute". The cross sections of nuclear reactions were measured by the stack foil technique, detecting the gamma radiation of the activation products. Gd, Tb, and Dy were separated by extraction chromatography using the LN Resin sorbent in nitric media. The isolated dysprosium fraction was stored for a day, and the formed ¹⁵⁵Tb was isolated by the same method.

Results: The cross sections for the formation of ¹⁵⁹Gd, ^153-156Tb, and ^155,157Dy under irradiation by alpha particles of a gadolinium target of natural isotopic composition in the energy range 20-60 MeV have been measured. The ¹⁵⁵Dy yield on a thick target at 60 MeV was 35 MBq/μAh, which makes it possible to obtain 1 GBq ¹⁵⁵Tb as a result of 12-hour irradiation with a beam current of 50 μA. Extraction chromatography on LN Resin sorbent in nitric enabled quick and efficient separation of Gd, Tb, and Dy. The radiochemical yield of Dy was 95%, for Tb > 95%. The main radionuclidic impurity is ¹⁵³Tb (T_1/2 = 2.34 d; <5.4% of ¹⁵⁵Tb activity).

Conclusions: The developed method allows the production of therapeutic amounts of ¹⁵⁵Tb with acceptable radionuclidic purity without the need for isotopically enriched materials. The amount of ¹⁵⁵Tb is sufficient for its use in Auger therapy, as well as for preclinical studies of the suitability of SPECT preparations in laboratory animals. Nevertheless, to obtain higher activities, a longer irradiation time and a higher projectile current are proposed. The ¹⁵³Tb radionuclide present in the final preparation has a shorter half-life than the target radionuclide, and its hard γ-lines have a probability of emission of less than 1%, from which it can be concluded that the negative effect will not be significant. However, a product of this purity and type of contamination requires additional testing for toxicity in living organisms. The final sample also includes a certain amount of ¹⁵⁷Tb (T_1/2 = 71 a, the only γ-line 54.5 keV Iγ = 0.0084%), which will complicate the labeling conditions. Thus, more research is needed in the labeling area. It should be noted that the use of gadolinium enriched in the ¹⁵⁵Gd or ¹⁵⁶Gd nuclide as a target will help not only reduce the amount of impurities but also increase the yield of ¹⁵⁵Tb.

Keywords: Cross section; Cyclotron; Nuclear reaction; Radiochemical separation; Terbium-155.