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Title: GLASS FABRICATION AND PRODUCT CONSISTENCY TESTING OF LANTHANIDE BOROSHILICATE FRIT X COMPOSITION FOR PLUTONIUM DISPOSITION

Technical Report ·
DOI:https://doi.org/10.2172/898365· OSTI ID:898365

The Department of Energy Office of Environmental Management (DOE/EM) plans to conduct the Plutonium Disposition Project at the Savannah River Site (SRS) to disposition excess weapons-usable plutonium. A plutonium glass waste form is the preferred option for immobilization of the plutonium for subsequent disposition in a geologic repository. A reference glass composition (Lanthanide Borosilicate (LaBS) Frit B) was developed during the Plutonium Immobilization Program (PIP) to immobilize plutonium in the late 1990's. A limited amount of performance testing was performed on this baseline composition before efforts to further pursue Pu disposition via a glass waste form ceased. Recent FY05 studies have further investigated the LaBS Frit B formulation as well as development of a newer LaBS formulation denoted as LaBS Frit X. The objectives of this present task were to fabricate plutonium loaded LaBS Frit X glass and perform corrosion testing to provide near-term data that will increase confidence that LaBS glass product is suitable for disposal in the Yucca Mountain Repository. Specifically, testing was conducted in an effort to provide data to Yucca Mountain Project (YMP) personnel for use in performance assessment calculations. Plutonium containing LaBS glass with the Frit X composition with a 9.5 wt% PuO{sub 2} loading was prepared for testing. Glass was prepared to support Product Consistency Testing (PCT) at Savannah River National Laboratory (SRNL). The glass was thoroughly characterized using x-ray diffraction (XRD) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS) prior to performance testing. A series of PCTs were conducted at SRNL using quenched Pu Frit X glass with varying exposed surface areas. Effects of isothermal and can-in-canister heat treatments on the Pu Frit X glass were also investigated. Another series of PCTs were performed on these different heat-treated Pu Frit X glasses. Leachates from all these PCTs were analyzed to determine the dissolved concentrations of key elements. Acid stripping of leach vessels was performed to determine the concentration of the glass constituents that may have sorbed on the vessels during leach testing. Additionally, the leachate solutions were ultrafiltered to quantify colloid formation. Characterization of the quenched Pu Frit X glass prior to testing revealed that some crystalline plutonium oxide was present in the glass. The crystalline particles had a disklike morphology and likely formed via coarsening of particles in areas compositionally enriched in plutonium. Similar results had also been observed in previous Pu Frit B studies. Isothermal 1250 C heat-treated Pu Frit X glasses showed two different crystalline phases (PuO{sub 2} and Nd{sub 2}Hf{sub 2}O{sub 7}), as well as a peak shift in the XRD spectra that is likely due to a solid solution phase PuO{sub 2}-HfO{sub 2} formation. Micrographs of this glass showed a clustering of some of the crystalline phases. Pu Frit X glass subjected to the can-in-canister heating profile also displayed the two PuO{sub 2} and Nd{sub 2}Hf{sub 2}O{sub 7} phases from XRD analysis. Additional micrographs indicate crystalline phases in this glass were of varying forms (a spherical PuO{sub 2} phase that appeared to range in size from submicron to {approx}5 micron, a dendritic-type phase that was comprised of mixed lanthanides and plutonium, and a minor phase that contained Pu and Hf), and clustering of the phases was also observed.

Research Organization:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
DE-AC09-96SR18500
OSTI ID:
898365
Report Number(s):
WSRC-STI-2006-00318; TRN: US0701902
Country of Publication:
United States
Language:
English