Distribution and Solubility of Radionuclides and Neutron Absorbers in Waste Forms for Disposition of Plutonium Ash and Scraps, Excess Plutonium, and Miscellaneous Spent Nuclear Fuels Page: 4 of 17
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hafnium, the hafnium oxide appears to be associated with the silica lattice rather than the boron-rich
areas.
This suggests that the two chemical forms of plutonium behave much different in glasses. For
example, at low sodium, essentially no hafnium oxide could be incorporated into the glasses. At low
sodium, additions of gadolinium oxide resulted in high melting glasses with precipitates. Adding
additional gadolinium oxide to the mix eventually yielded clear glasses. Therefore, it is anticipated that
the +3 oxidation state of plutonium is more soluble than the +4 oxidation state. Preliminary data suggest
this to be the case.
Actual work with plutonium was to start in the third year of the project. We began the process of
obtaining the plutonium in the forth quarter of the second year. It took one year to obtain the necessary
plutonium. This left little time to perform any experiments. We prepared about ten glasses. We used our
models based on our results with gadolinium and hafnium to calculate the expected solubility limits for
the plutonium oxide. We were in the process of characterizing one of these samples when the analyst
inadvertently touched the glass specimen with the microscope lens. The amount of plutonium released
was small, weighing approximately 1 microgram. The resulting effort to remove the contamination from
the laboratory consumed the remaining funds, and the characterization was never completed. Fortunately,
the personnel in the laboratory at the time did not receive any plutonium internally or externally.
In the course of analyzing the data from the gadolinium oxide and hafnium oxide-containing glasses,
a model for the solubility of these oxides in glasses was developed. At the time the project ended, the
model was being generalized so that it would be applicable to other metal oxides. This was the subject of
a proposal for additional EMSP funds to continue the development, but this was an unsuccessful attempt.
Had this proposal been funded, we feel certain that the model would allow us to put glass development on1V
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Strachan, Dr. Denis M.; Shuh, Dr. David K.; Ewing, Dr. Rodney C. & Vance, Dr. Eric R. Distribution and Solubility of Radionuclides and Neutron Absorbers in Waste Forms for Disposition of Plutonium Ash and Scraps, Excess Plutonium, and Miscellaneous Spent Nuclear Fuels, report, September 23, 2002; United States. (https://digital.library.unt.edu/ark:/67531/metadc733371/m1/4/: accessed April 24, 2024), University of North Texas Libraries, UNT Digital Library, https://digital.library.unt.edu; crediting UNT Libraries Government Documents Department.