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Title: Results of an inter-laboratory study of glass formulation for the immobilization of excess plutonium

Abstract

The primary focus of the current study is to determine allowable loadings of feed streams containing different ratios of plutonium, uranium, and minor components into the LaBS glass and to evaluate thermal stability with respect to the DWPF pour.

Authors:
Publication Date:
Research Org.:
Savannah River Site (US)
Sponsoring Org.:
US Department of Energy (US)
OSTI Identifier:
750083
Report Number(s):
SRT-PUM-97-0017
TRN: US0001327
DOE Contract Number:
AC09-96SR18500
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: 8 Dec 1999
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 36 MATERIALS SCIENCE; PLUTONIUM; URANIUM; LOADING RATE; WASTE FORMS; GLASS; INTERLABORATORY COMPARISONS; VITRIFICATION; RADIOACTIVE WASTE DISPOSAL; THERMODYNAMIC PROPERTIES

Citation Formats

Peeler, D.K. Results of an inter-laboratory study of glass formulation for the immobilization of excess plutonium. United States: N. p., 1999. Web. doi:10.2172/750083.
Peeler, D.K. Results of an inter-laboratory study of glass formulation for the immobilization of excess plutonium. United States. doi:10.2172/750083.
Peeler, D.K. Wed . "Results of an inter-laboratory study of glass formulation for the immobilization of excess plutonium". United States. doi:10.2172/750083. https://www.osti.gov/servlets/purl/750083.
@article{osti_750083,
title = {Results of an inter-laboratory study of glass formulation for the immobilization of excess plutonium},
author = {Peeler, D.K.},
abstractNote = {The primary focus of the current study is to determine allowable loadings of feed streams containing different ratios of plutonium, uranium, and minor components into the LaBS glass and to evaluate thermal stability with respect to the DWPF pour.},
doi = {10.2172/750083},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Wed Dec 08 00:00:00 EST 1999},
month = {Wed Dec 08 00:00:00 EST 1999}
}

Technical Report:

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  • This report summarizes our findings from pressurized unsaturated flow (PUF) and single-pass flow-through (SPFT) experiments to date. Results from the PUF test of a Pu-bearing ceramic with enclosing surrogate high-level waste glass show that the glass reacts rapidly to alteration products. Glass reaction causes variations in the solution pH in contact with the ceramic materials. We also document variable concentrations of Pu in solution, primarily in colloidal form, which appear to be related to secular variations in solution composition. The apparent dissolution rate of the ceramic waste form, based on Ba concentrations in the effluent, is estimated at {le} 10{supmore » {minus}5} g/(m{sup 2} {center_dot} d). Pu-bearing colloids were recovered in the size range of 0.2 to 2 {micro}m, but it is not clear that such entities would be transported in a system that is not advective-flow dominated. Results from SPFT experiments give information on the corrosion resistance of two surrogate Pu-ceramics (Ce-pyrochlore and Ce-zirconolite) at 90 C over a pH range of 2 to 12. The two ceramics were doped with minor quantities ({approximately}0.1 mass%) of MoO{sub 3}, so that concentrations of Mo in the effluent solution could be used to monitor the reaction behavior of the materials. The data obtained thus far from experiments with durations up to 150 d do not conclusively prove that the solid-aqueous solution systems have reached steady-state conditions. Therefore, the dissolution mechanism cannot be determined. Apparent dissolution rates of the two ceramic materials based on Ce, Gd, and Mo concentrations in the effluent solutions from the SPFT are nearly identical and vary between 1.1 to 8.5 x 10{sup {minus}4} g/(m{sup 2} {center_dot} d). In addition, the data reveal a slightly amphoteric dissolution behavior, with a minimum apparent rate at pH = 7 to 8, over the pH range examined. Results from two related ceramic samples suggest that radiation damage can have a measurable effect on the dissolution of titanium-based ceramics. The rare earth pyrochlores, Gd{sub 2}Ti{sub 2}O{sub 7} and Lu{sub 2}Ti{sub 2}O{sub 7}, are being studied as part of the DOE Environmental Management Science Program, and the results are germane to this study. The corrosion resistances of both heavy-ion bombarded and pristine (non-bombarded) specimens are being examined with the SPFT test. Initial data indicate that the dissolution rate may increase by a factor of 3 times or more when these materials become amorphous from radiation damage.« less
  • This document presents the differences between two HLW glass formulation models (GFM): The 1996 GFM and 2009 GFM. A glass formulation model is a collection of glass property correlations and associated limits, as well as model validity and solubility constraints; it uses the pretreated HLW feed composition to predict the amount and composition of glass forming additives necessary to produce acceptable HLW glass. The 2009 GFM presented in this report was constructed as a nonlinear optimization calculation based on updated glass property data and solubility limits described in PNNL-18501 (2009). Key mission drivers such as the total mass of HLWmore » glass and waste oxide loading are compared between the two glass formulation models. In addition, a sensitivity study was performed within the 2009 GFM to determine the effect of relaxing various constraints on the predicted mass of the HLW glass.« less
  • The joint goal of the Russian work is to establish a full-scale plutonium immobilization facility at a Russian industrial site by 2005. To achieve this requires that the necessary engineering and technical basis be developed in these Russian projects and the needed Russian approvals be obtained to conduct industrial-scale immobilization of plutonium-containing materials at a Russian industrial site by the 2005 date. This meeting and future work will provide the basis for joint decisions. Supporting R&D projects are being carried out at Russian Institutes that directly support the technical needs of Russian industrial sites to immobilize plutonium-containing materials. Special R&Dmore » on plutonium materials is also being carried out to support excess weapons disposition in Russia and the US, including nonproliferation studies of plutonium recovery from immobilization forms and accelerated radiation damage studies of the US-specified plutonium ceramic for immobilizing plutonium. This intriguing and extraordinary cooperation on certain aspects of the weapons plutonium problem is now progressing well and much work with plutonium has been completed in the past two years. Because much excellent and unique scientific and engineering technical work has now been completed in Russia in many aspects of plutonium immobilization, this meeting in St. Petersburg was both timely and necessary to summarize, review, and discuss these efforts among those who performed the actual work. The results of this meeting will help the US and Russia jointly define the future direction of the Russian plutonium immobilization program, and make it an even stronger and more integrated Russian program. The two objectives for the meeting were to: (1) Bring together the Russian organizations, experts, and managers performing the work into one place for four days to review and discuss their work with each other; and (2) Publish a meeting summary and a proceedings to compile reports of all the excellent Russian plutonium immobilization contract work. This proceedings document presents the wide extent of Russian immobilization activities, provides a reference for their work, and makes it available to others.« less
  • A key milestone for the Immobilization Project (AOP Milestone 3.2a) in Fiscal Year 1998 (FY98) is the definition of the baseline composition or formulation for the plutonium ceramic form. The baseline formulation for the plutonium ceramic product must be finalized before the repository- and plant-related process specifications can be determined. The baseline formulation that is currently specified is given in Table 1.1. In addition to the baseline formulation specification, this report provides specifications for two alternative formulations, related compositional specifications (e.g., precursor compositions and mixing recipes), and other preliminary form and process specifications that are linked to the baseline formulation.more » The preliminary specifications, when finalized, are not expected to vary tremendously from the preliminary values given.« less