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  1. Nuclear data for reactor production of 131Ba and 133Ba

    The newest radioisotope for brachytherapy treatment of prostate cancer is 131Cs (t1/2 = 9.69 d, 100% EC). Generated via electron capture decay of 131Ba (t1/2 = 11.6 d, 100% EC), 131Cs has been used in brachytherapy for prostate cancer since 2004. The 131Ba parent is produced through neutron capture of enriched 130Ba in a nuclear reactor. For large-scale production of 131Ba, an accurate knowledge of production and burnup cross sections of 131Ba are essential. Here, we report two group cross sections (thermal and resonance integrals) for 130Ba and 131Ba and a new measure of the half-life of 131Ba. Targets consistingmore » of milligram quantities of enriched 130Ba (~35%) were irradiated in Oak Ridge National Laboratory's High Flux Isotope Reactor at thermal and resonance neutron fluxes of (1.9–2.1) × 1015 and (5.8–7.0) × 1013 neutrons·cm-2 s-1, respectively, for durations ranging from 3 to 26 days. In addition, cadmium covered samples of 130Ba were irradiated for 1 hour at 12.6% full reactor power (10.7 MW). The yield of 131Ba approaches a saturation value of ~60 GBq (~1.6 Ci) per mg of 130Ba for 20 days irradiation at a thermal neutron flux of 1.8 × 1015 n·s-1·cm-2, with a thermal/epithermal ratio of ~30. Under the above experimental conditions, the two group cross sections of 130Ba are 6.9 ± 0.5 b (thermal, σ0) and 173 ± 7 b (resonance, I0). These values represent the sum of cross sections to metastable and ground states of 131Ba. For 131Ba, the empirically measured thermal cross section is 200 ± 50 b assuming an I00 of 10. This cross section is reported for the first time. Further, the half-life of 131Ba was remeasured to be 11.657 ± 0.008 d. Lastly, this study also resulted in the co-production of 133Ba (t1/2 = 10.52 y, 100% EC). The experimental yield of 133Ba is ~370 MBq (~10 mCi) per mg of 132Ba (thin target) for one cycle irradiation in the High Flux Isotope Reactor, and measured two-group 132Ba cross sections are 7.2 ± 0.2 b and 39.9 ± 1.3 b. These values also represent the sum of cross sections to metastable and ground states of 133Ba.« less
  2. Multifunctional GdVO4: Eu core–shell nanoparticles containing 225Ac for targeted alpha therapy and molecular imaging

    Gadolinium vanadate nanoparticles (NPs) doped with europium, in concentrations between 5–40%, were synthesized via an aqueous route to prove their multimodal imaging functionalities and their performance as radionuclide carriers for targeted alpha therapy. Core–shell Gd0.8Eu0.2VO4 NPs were doped with the α-emitting actinium-225 to assess the in vitro retention of 225Ac and its decay daughters; francium-221 and bismuth-213. Gd0.8Eu0.2VO4 core–shell NPs were obtained using a precipitation synthesis route having a tetragonal system, a spherical morphology, and a uniform particle size distribution. Gd0.8Eu0.2VO4 core–shell NPs displayed the characteristic intense emission at 618 nm (red) and paramagnetic behavior of Eu and Gd cations,more » respectively. Partial retention of radionuclides was obtained with Gd0.8Eu0.2VO4 core NPs, while deposition of two nonradioactive Gd0.8Eu0.2VO4 shells significantly decreased the leakage of both 225Ac and 221Fr. As a result, the luminescence and magnetic functionalities as well as radionuclide retention capabilities of Gd0.8Eu0.2VO4 core–shell NPs demonstrate their potential for biomedical applications.« less
  3. Synthesis and characterization of intrinsically radiolabeled lanthanide phosphate nanoparticles toward biomedical and environmental applications

    Lanthanide phosphate nanomaterials are appealing as multifunctional platforms for biomedical applications because of their low toxicity, radiation resistance, and unique luminescence and magnetic properties. Lanthanide phosphate nanoparticles (NPs) radiolabeled with 156Eu were synthesized by an aqueous route using sodium tripolyphosphate as a phosphate source and complexing agent. GdPO4 was used as a host matrix, while synthetic concentrations of Ce3+/Tb3+ and Eu3+ were varied between 5–40% and 10–30%, respectively, and yielded spherical NPs with hexagonal crystal system and particle size < 5 nm. Luminescence emission and magnetic susceptibility were influenced by lanthanide concentrations where characteristic 5D0-7FJ and 5D4-7FJ transitions were observedmore » for Eu3+- and Tb3+-doped NPs, respectively. Chemical yield of > 90% was achieved for GdPO4 and Gd0.6Ce0.3Tb0.1PO4 NPs intrinsically radiolabeled with 156Eu. Lastly, in vitro retention of 156Eu within LnPO4 NPs was > 97% over 3 weeks. Intrinsically radiolabeled LnPO4 NPs have the potential to combine the luminescence and magnetic properties of Ln3+ ions with lanthanide radioisotopes for biomedical and environmental applications.« less
  4. Simultaneous Separation of Actinium and Radium Isotopes from a Proton Irradiated Thorium Matrix

    A new method has been developed for the isolation of 223,224,225Ra, in high yield and purity, from a proton irradiated 232Th matrix. We report an all-aqueous process using multiple solid-supported adsorption steps including a citrate chelation method developed to remove >99.9% of the barium contaminants by activity from the final radium product. Moreover, we developed a procedure involving the use of three columns in succession, and the separation of 223,224,225Ra from the thorium matrix was obtained with an overall recovery yield of 91 ± 3%, average radiochemical purity of 99.9%, and production yields that correspond to physical yields based onmore » previously measured excitation functions.« less
  5. Automated cassette-based production of high specific activity [203/212Pb]peptide-based theranostic radiopharmaceuticals for image-guided radionuclide therapy for cancer

    A method for preparation of Pb-212 and Pb-203 labeled chelator-modified peptide-based radiopharmaceuticals for cancer imaging and radionuclide therapy has been developed and adapted for automated clinical production. Pre-concentration and isolation of radioactive Pb2+ from interfering metals in dilute hydrochloric acid was optimized using a commercially-available Pb-specific chromatography resin packed in disposable plastic columns. The pre-concentrated radioactive Pb2+ is eluted in NaOAc buffer directly to the reaction vessel containing chelator-modified peptides. Radiolabeling was found to proceed efficiently at 85 °C (45 min; pH 5.5). The specific activity of radiolabeled conjugates was optimized by separation of radiolabeled conjugates from unlabeled peptide viamore » HPLC. Preservation of bioactivity was confirmed by in vivo biodistribution of Pb-203 and Pb-212 labeled peptides in melanoma-tumor-bearing mice. The approach has been found to be robustly adaptable to automation and a cassette-based fluid-handling system (Modular Lab Pharm Tracer) has been customized for clinical radiopharmaceutical production. Our findings demonstrate that the Pb-203/Pb-212 combination is a promising elementally-matched radionuclide pair for image-guided radionuclide therapy for melanoma, neuroendocrine tumors, and potentially other cancers.« less

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