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Dissertation
Antimony-119 for Radiopharmaceutical Therapy
2024
Overview
This dissertation investigates production, chemical isolation, and radiopharmaceutical incorporation of the therapeutic radionuclide 119Sb (119Sb, t1/2 = 38.19 22 h, EC=100%) and its radioisotopic imaging analogue 117Sb (t1/2 = 2.80 1 h, EC = 100%, Eγ = 158.562 15 keV, Iγ = 85.9%, Eβ+ = 262.4 4 keV, Iβ+ = 1.81 11 %). For decades, researchers have predicted 119Sb to be one of the most promising Auger electron-emitting radionuclides for therapeutic application because of its high electron yield (~24 electrons per decay), optimal emitted internal conversion electron energies (20 – 30 keV), and low co-emission of photons (Emax = 29.1 keV, I = 2.18 7 %). Barriers in 119Sb production, chemical isolation from target material, and stable radiometal complexation with a bifunctional chelator have limited exploration of 119Sb’s therapeutic potential to in silico studies. This work begins by developing production and chemical isolation techniques, electroplating tin targets suitable for low energy proton and deuteron irradiation and separating Sb from Sn using column chromatography and liquid extraction. We discovered target recycling techniques compatible with our column-based Sn(II)/Sb(III) separation, allowing us to sustainably irradiate 96.3% isotopically enriched 119Sn to make radionuclidically pure 119Sb. With collaborators in inorganic chemistry, we found two chelators capable of bifunctionalization for complexing radioantimony—a trithiol chelator for complexing Sb(III) and a tris-catechol chelator (TREN-CAM) for Sb(V). Using spectroscopy, in vitro, in vivo, and ex vivo techniques, we characterized [nat/1XXSb]Sb-trithiol-diacid and [nat/1XXSb]Sb-TREN-CAM complexes, reported X-ray crystal structures, and analyzed complex stability. [nat/1XXSb]Sb-trithiol-diacid was stable in serum, but upon conjugation to a targeting moiety, the complexes decomposed in PBS. We collected the first in vivo PET and SPECT images of a chelator complexed radioactive antimony to prove [nat/1XXSb]Sb-TREN-CAM complex’s stability.
Publisher
ProQuest Dissertations & Theses
Subject
ISBN
9798346855125
