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1.
Inorg Chem ; 59(9): 6137-6146, 2020 May 04.
Artigo em Inglês | MEDLINE | ID: mdl-32302134

RESUMO

Increasing access to the short-lived α-emitting radionuclide astatine-211 (211At) has the potential to advance targeted α-therapeutic treatment of disease and to solve challenges facing the medical community. For example, there are numerous technical needs associated with advancing the use of 211At in targeted α-therapy, e.g., improving 211At chelates, developing more effective 211At targeting, and characterizing in vivo 211At behavior. There is an insufficient understanding of astatine chemistry to support these efforts. The chemistry of astatine is one of the least developed of all elements on the periodic table, owing to its limited supply and short half-life. Increasing access to 211At could help address these issues and advance understanding of 211At chemistry in general. We contribute here an extraction chromatographic processing method that simplifies 211At production in terms of purification. It utilizes the commercially available Pre-Filter resin to rapidly (<1.5 h) isolate 211At from irradiated bismuth targets (Bi decontamination factors ≥876 000), in reasonable yield (68-55%) and in a form that is compatible for subsequent in vivo study. We are excited about the potential of this procedure to address 211At supply and processing/purification problems.

2.
ACS Cent Sci ; 5(3): 494-505, 2019 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-30937377

RESUMO

Radionuclides find widespread use in medical technologies for treating and diagnosing disease. Among successful and emerging radiotherapeutics, 119Sb has unique potential in targeted therapeutic applications for low-energy electron-emitting isotopes. Unfortunately, developing 119Sb-based drugs has been slow in comparison to other radionuclides, primarily due to limited accessibility. Herein is a production method that overcomes this challenge and expands the available time for large-scale distribution and use. Our approach exploits high flux and fluence from high-energy proton sources to produce longer lived 119mTe. This parent isotope slowly decays to 119Sb, which in turn provides access to 119Sb for longer time periods (in comparison to direct 119Sb production routes). We contribute the target design, irradiation conditions, and a rapid procedure for isolating the 119mTe/119Sb pair. To guide process development and to understand why the procedure was successful, we characterized the Te/Sb separation using Te and Sb K-edge X-ray absorption spectroscopy. The procedure provides low-volume aqueous solutions that have high 119mTe-and consequently 119Sb-specific activity in a chemically pure form. This procedure has been demonstrated at large-scale (production-sized, Ci quantities), and the product has potential to meet stringent Food and Drug Administration requirements for a 119mTe/119Sb active pharmaceutical ingredient.

3.
Inorg Chem ; 53(23): 12315-22, 2014 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-25390284

RESUMO

Platinum group metals (PGMs), including rhodium, generated by the fission of (235)U are present in significant quantities within spent nuclear fuel located on power generation sites in the United States, the amount of which is expected to exceed natural reserves by 2030. Yet, spent fuel raffinates are highly acidic media that may result in complex speciation of the PGM. This work provides an understanding of Rh(III) speciation up to 9 M HCl and HNO3, and utilizes a combination of ultraviolet-visible (UV-vis) and capillary zone electrophoresis data, along with computationally predicted thermochemistry and simulated UV-vis spectra to approximate the relative concentrations of potential species in solution as a function of acid concentration. One Rh(III) species, [Rh(NO3)3], is observed under all conditions in HNO3 and for Rh(III) concentrations smaller than 10(-3) M. In contrast, a variety of chloridated Rh(III) species may exist simultaneously in a HCl medium. The species [RhCl2(H2O)4](+) and [RhCl3(H2O)3] are observed in HCl solutions of concentrations ranging from 0 to 1 M; the species [RhCl4(H2O)2](-), [RhCl5(H2O)](2-), and [Rh2Cl9](3-) are observed between 2 and 9 M HCl.

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