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Title: GLASS FABRICATION AND PRODUCT CONSISTENCY TESTING OF LANTHANIDE BOROSILICATE FRIT B COMPOSITION FOR PLUTONIUM DISPOSITION

Abstract

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 a leading candidate 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. 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. Therefore, the objectives of this present task were to fabricate plutonium loaded LaBS Frit B glass and perform additional 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 B 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) and for additional performance testing at Argonne National Laboratorymore » (ANL) and Pacific Northwest National Laboratory (PNNL). The glass was 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 with varying exposed surface area and test durations. The leachates from these tests 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. The leached solids from select PCTs were examined in an attempt to evaluate the Pu and neutron absorber release behavior from the glass and to identify the formation of alteration phases on the glass surface. Characterization of the glass prior to testing revealed that some undissolved plutonium oxide was present in the glass. The undissolved particles had a disk-like morphology and likely formed via coarsening of particles in areas compositionally enriched in plutonium. Similar disk-like PuO{sub 2} phases were observed in previous LaBS glass testing at PNNL. In that work, researchers concluded that plutonium formed with this morphology as a result of the leaching process. It was more likely that the presence of the plutonium oxide crystals in the PNNL testing was a result of glass fabrication. A series of PCTs were conducted at 90 C in ASTM Type 1 water. The PCT-Method A (PCT-A) was conducted to compare the Pu LaBS Frit B glass durability to current requirements for High Level Waste (HLW) glass in a geologic repository. The PCT-A test has a strict protocol and is designed to specifically be used to evaluate whether the chemical durability and elemental release characteristics of a nuclear waste glass have been consistently controlled during production and, thus, meet the repository acceptance requirements. The PCT-A results on the Pu containing LaBS Frit B glass showed that the glass was very durable with a normalized elemental release value for boron of approximately 0.02 g/L. This boron release value was better than two orders of magnitude better from a boron release standpoint than the current Environmental Assessment (EA) glass used for repository acceptance. The boron release value for EA glass is 16.7 g/L.« less

Authors:
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
897869
Report Number(s):
WSRC-TR-2006-00033
TRN: US0701523
DOE Contract Number:  
DE-AC09-96SR18500
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; BOROSILICATE GLASS; FABRICATION; GLASS; NEUTRON ABSORBERS; PERFORMANCE TESTING; PLUTONIUM; PLUTONIUM OXIDES; RADIOACTIVE WASTES; RARE EARTHS; SCANNING ELECTRON MICROSCOPY; SURFACE AREA; TESTING; WASTE FORMS; X-RAY DIFFRACTION; YUCCA MOUNTAIN

Citation Formats

Marra, J. GLASS FABRICATION AND PRODUCT CONSISTENCY TESTING OF LANTHANIDE BOROSILICATE FRIT B COMPOSITION FOR PLUTONIUM DISPOSITION. United States: N. p., 2006. Web. doi:10.2172/897869.
Marra, J. GLASS FABRICATION AND PRODUCT CONSISTENCY TESTING OF LANTHANIDE BOROSILICATE FRIT B COMPOSITION FOR PLUTONIUM DISPOSITION. United States. https://doi.org/10.2172/897869
Marra, J. 2006. "GLASS FABRICATION AND PRODUCT CONSISTENCY TESTING OF LANTHANIDE BOROSILICATE FRIT B COMPOSITION FOR PLUTONIUM DISPOSITION". United States. https://doi.org/10.2172/897869. https://www.osti.gov/servlets/purl/897869.
@article{osti_897869,
title = {GLASS FABRICATION AND PRODUCT CONSISTENCY TESTING OF LANTHANIDE BOROSILICATE FRIT B COMPOSITION FOR PLUTONIUM DISPOSITION},
author = {Marra, J},
abstractNote = {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 a leading candidate 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. 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. Therefore, the objectives of this present task were to fabricate plutonium loaded LaBS Frit B glass and perform additional 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 B 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) and for additional performance testing at Argonne National Laboratory (ANL) and Pacific Northwest National Laboratory (PNNL). The glass was 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 with varying exposed surface area and test durations. The leachates from these tests 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. The leached solids from select PCTs were examined in an attempt to evaluate the Pu and neutron absorber release behavior from the glass and to identify the formation of alteration phases on the glass surface. Characterization of the glass prior to testing revealed that some undissolved plutonium oxide was present in the glass. The undissolved particles had a disk-like morphology and likely formed via coarsening of particles in areas compositionally enriched in plutonium. Similar disk-like PuO{sub 2} phases were observed in previous LaBS glass testing at PNNL. In that work, researchers concluded that plutonium formed with this morphology as a result of the leaching process. It was more likely that the presence of the plutonium oxide crystals in the PNNL testing was a result of glass fabrication. A series of PCTs were conducted at 90 C in ASTM Type 1 water. The PCT-Method A (PCT-A) was conducted to compare the Pu LaBS Frit B glass durability to current requirements for High Level Waste (HLW) glass in a geologic repository. The PCT-A test has a strict protocol and is designed to specifically be used to evaluate whether the chemical durability and elemental release characteristics of a nuclear waste glass have been consistently controlled during production and, thus, meet the repository acceptance requirements. The PCT-A results on the Pu containing LaBS Frit B glass showed that the glass was very durable with a normalized elemental release value for boron of approximately 0.02 g/L. This boron release value was better than two orders of magnitude better from a boron release standpoint than the current Environmental Assessment (EA) glass used for repository acceptance. The boron release value for EA glass is 16.7 g/L.},
doi = {10.2172/897869},
url = {https://www.osti.gov/biblio/897869}, journal = {},
number = ,
volume = ,
place = {United States},
year = {2006},
month = {1}
}