Introduction
Rhenium-186 (t1/2 = 3.72 d) is very attractive for use as a theranostic agent in targeted radionuclide therapy (Eβ max = 1.072 MeV (> 76.6 %); Eγ = 137.2 keV)1. Previously published investigations of high specific activity 186Re production have utilized the 186W(p,n)186Re or 186W(d,2n)186Re reactions2-5. Our group is interested in the refinement and scale-up of the production of high specific activity 186Re by cyclotron irradiations of 186W with deuterons; including investigations of the most suitable target material. WO3 has been successfully used as a target material in proton irradiations by two other groups4,5. Further, the physical properties of WO3, such as the reported monoclinic with Pc space group, body centered cubic crystal structure6 and melting point of 1473 °C, made for an attractive target material as sintered and other more structurally robust pressed pellet target preparations could be explored. Thus, this study reports on the characterization and suitability of WO3 as a full-thickness target material for the deuteron production of 186Re.
Materials and Methods
Assessments of WO3 for target material suitability and structural integrity were made on thick targets (~1 g) prepared using both commercially available and converted WO3 by either uniaxially pressing (13.8 MPa) of powdered WO3 into an aluminum target support or by placing sintered WO3 pellets (1105 °C for 12 hours) into an aluminum target support.
In some experiments, WO3 pellets were prepared by dissolution of Wmetal with H2O2, then treatment with 1.5 M HCl. The recovered hydrated WO3 was calcinated at 800 °C for 4 hours, allowed to cool to ambient temperature, pulverized with a mortar and pestle, uniaxially pressed at 13.8 MPa into pellets with a 13 mm die, and subsequently sintered in a tube furnace under flowing Ar at 1105 °C for 3, 6, and 12 hours. Material characterization and product composition analyses were conducted with SEM, EDS, XRD, Raman spectroscopy, and visible photoluminescence spectroscopy.
Thick WO3 targets were irradiated for 10 min at 10 µA with nominal extracted deuteron energies of 17 MeV. Gamma-ray spectroscopy was per-formed to assess production yields and radionuclidic byproducts at least 24 hours post EOB.
Results
While the color of the commercially available WO3 is slightly different (dull, pale green) than the brighter more yellow color of the chemically processed WO3, X-ray diffraction spectrometry (XRD) indicated the two samples were virtually identical.
Attempts to determine how the duration of the sintering process (at 1105 °C) affects the chemical/physical nature of the pellet yielded surprising results. In contrast to the characteristic annealed appearance of sintered material, grains of the WO3 sample appeared more densely packed, but not sintered to one another as had been seen during higher temperature (1550 °C) reductions of WO3 irrespective of the time interval used.
Full-thickness pressed or sintered pellets of WO3 were found to disintegrate upon irradiation with the deuteron beam, allowing for the direct irradiation of the aluminum target body producing 24Na as a contaminant. Upon retrieval of the target support it was observed that the WO3 had vaporized, discoloring the surface of the well in the target support and coating the walls of ~61 cm (24 inches) of the terminal portion of the beamline, which then required decontamination. We believe that these observations are the result of outgassing oxygen species that subsequently reacted with the aluminum target support. While these findings are in sharp contrast with the successful production yields and isolations previously reported by both Shigeta et al. and Fassbender et al., we believe that these differences are attributable to differences in target design (previous studies utilized an en-closed target with cooling in front of and behind the target) necessitated by the configuration of our target station.
Conclusions.
The physical properties of powdered WO3, including its lower melting point and more suitable compressibility than powdered Wmetal, seemed to enhance the structural integrity of a WO3 pellet (whether pressed or sintered). However, when compared to our recent successes with the use of Wmetal based targets, the disappointing degradation of our WO3 targets when irradiated with the incident deuteron beam has led us to believe that Wmetal is the more viable target material for 186Re production in our facility.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:22232 |
| Date | January 2015 |
| Creators | Balkin, E. R., Strong, K. T., Smith, B. E., Gagnon, K., Dorman, E., Emery, R., Pauzauskie, P., Fassbender, M. E., Cutler, C. S., Ketring, A. R., Jurisson, S. S., Wilbur, D. S. |
| Contributors | University of Washington, Seattle, USA, Los Alamos National Laboratory, Los Alamos, USA, University of Missouri, Columbia, USA |
| Publisher | Helmholtz-Zentrum Dresden - Rossendorf |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | doc-type:conferenceObject, info:eu-repo/semantics/conferenceObject, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | urn:nbn:de:bsz:d120-qucosa-162048, qucosa:22221 |
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