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.
Radionuclides find
widespread use in medical technologies for treating
and diagnosing disease. Among successful and emerging radiotherapeutics,
119
Sb has unique potential in targeted therapeutic applications
for low-energy electron-emitting isotopes. Unfortunately, developing
119
Sb-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
119m
Te. This parent isotope slowly decays to
119
Sb, which
in turn provides access to
119
Sb for longer time periods
(in comparison to direct
119
Sb production routes). We contribute
the target design, irradiation conditions, and a rapid procedure for
isolating the
119m
Te/
119
Sb 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
119m
Te—and consequently
119
Sb—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
119m
Te/
119
Sb active pharmaceutical
ingredient.
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.
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