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Title: Glass binder development for a glass-bonded sodalite ceramic waste form

Abstract

This paper discusses work to develop Na2O-B2O3-SiO2 glass binders for immobilizing LiCl-KCl eutectic salt waste in a glass-bonded sodalite waste form following electrochemical reprocessing of used metallic nuclear fuel. Here, five new glasses with high Na2O contents were designed to generate waste forms having higher sodalite contents and fewer stress fractures. The structural, mechanical, and thermal properties of the new glasses were measured using variety of analytical techniques. The glasses were then used to produce ceramic waste forms with surrogate salt waste. The materials made using the glasses developed during this study were formulated to generate more sodalite than materials made with previous baseline glasses used. The coefficients of thermal expansion for the glass phase in the glass-bonded sodalite waste forms made with the new binder glasses were closer to the sodalite phase in the critical temperature region near and below the glass transition temperature. These improvements should result in lower probability of cracking in the full-scale monolithic ceramic waste form, leading to better long-term chemical durability. Additionally, a model generated during this study for predicting softening temperature of silicate binder glasses is presented.

Authors:
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Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1371995
Report Number(s):
PNNL-SA-123338
Journal ID: ISSN 0022-3115; AF5805020
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Nuclear Materials; Journal Volume: 489; Journal Issue: C
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; Sodalite-Bearing Ceramic Waste Form; sodalite; electrochemical; glass binder

Citation Formats

Riley, Brian J., Vienna, John D., Frank, Steven M., Kroll, Jared O., Peterson, Jacob A., Canfield, Nathan L., Zhu, Zihua, Zhang, Jiandong, Kruska, Karen, Schreiber, Daniel K., and Crum, Jarrod V.. Glass binder development for a glass-bonded sodalite ceramic waste form. United States: N. p., 2017. Web. doi:10.1016/j.jnucmat.2017.03.041.
Riley, Brian J., Vienna, John D., Frank, Steven M., Kroll, Jared O., Peterson, Jacob A., Canfield, Nathan L., Zhu, Zihua, Zhang, Jiandong, Kruska, Karen, Schreiber, Daniel K., & Crum, Jarrod V.. Glass binder development for a glass-bonded sodalite ceramic waste form. United States. doi:10.1016/j.jnucmat.2017.03.041.
Riley, Brian J., Vienna, John D., Frank, Steven M., Kroll, Jared O., Peterson, Jacob A., Canfield, Nathan L., Zhu, Zihua, Zhang, Jiandong, Kruska, Karen, Schreiber, Daniel K., and Crum, Jarrod V.. Thu . "Glass binder development for a glass-bonded sodalite ceramic waste form". United States. doi:10.1016/j.jnucmat.2017.03.041.
@article{osti_1371995,
title = {Glass binder development for a glass-bonded sodalite ceramic waste form},
author = {Riley, Brian J. and Vienna, John D. and Frank, Steven M. and Kroll, Jared O. and Peterson, Jacob A. and Canfield, Nathan L. and Zhu, Zihua and Zhang, Jiandong and Kruska, Karen and Schreiber, Daniel K. and Crum, Jarrod V.},
abstractNote = {This paper discusses work to develop Na2O-B2O3-SiO2 glass binders for immobilizing LiCl-KCl eutectic salt waste in a glass-bonded sodalite waste form following electrochemical reprocessing of used metallic nuclear fuel. Here, five new glasses with high Na2O contents were designed to generate waste forms having higher sodalite contents and fewer stress fractures. The structural, mechanical, and thermal properties of the new glasses were measured using variety of analytical techniques. The glasses were then used to produce ceramic waste forms with surrogate salt waste. The materials made using the glasses developed during this study were formulated to generate more sodalite than materials made with previous baseline glasses used. The coefficients of thermal expansion for the glass phase in the glass-bonded sodalite waste forms made with the new binder glasses were closer to the sodalite phase in the critical temperature region near and below the glass transition temperature. These improvements should result in lower probability of cracking in the full-scale monolithic ceramic waste form, leading to better long-term chemical durability. Additionally, a model generated during this study for predicting softening temperature of silicate binder glasses is presented.},
doi = {10.1016/j.jnucmat.2017.03.041},
journal = {Journal of Nuclear Materials},
number = C,
volume = 489,
place = {United States},
year = {Thu Jun 01 00:00:00 EDT 2017},
month = {Thu Jun 01 00:00:00 EDT 2017}
}
  • This paper discusses work to develop Na 2O-B 2O 3-SiO 2 glass binders for immobilizing LiCl-KCl eutectic salt waste in a glass-bonded sodalite waste form following electrochemical reprocessing of used metallic nuclear fuel. In this paper, five new glasses with ~20 mass% Na 2O were designed to generate waste forms with high sodalite. The glasses were then used to produce ceramic waste forms with a surrogate salt waste. The waste forms made using these new glasses were formulated to generate more sodalite than those made with previous baseline glasses for this type of waste. The coefficients of thermal expansion formore » the glass phase in the glass-bonded sodalite waste forms made with the new binder glasses were closer to the sodalite phase in the critical temperature region near and below the glass transition temperature than previous binder glasses used. Finally, these improvements should result in lower probability of cracking in the full-scale monolithic ceramic waste form, leading to better long-term chemical durability.« less
  • A glass bonded-sodalite ceramic waste form (CWF) has been developed to immobilize salt wastes from electrometallurgical treatment of sodium-bonded spent nuclear fuel. The CWF is a composite of salt-loaded sodalite and a binder glass formed at high temperature (850-950 C) by hot isostatic pressing (HIP) or pressureless-consolidation (PC) processes. A waste form degradation and radionuclide release model has been developed to support qualification of the CWF for disposal in the proposed repository at Yucca Mountain. Six series of tests were conducted in conjunction with the development of that model. (1) Static tests were conducted to measure the dissolution rate ofmore » sodalite, HIP binder glass, and HIP CWF at 40, 70, and 90 C in pH range 4.8-9.8 buffer solution. The parameter values in the degradation model were calculated from the dissolution rates measured by the static tests. (2) Static tests were conducted at 70 C in noncomplexing tertiary amine pH buffers to confirm that the dissolution rate measured with traditional buffers was not affected by the complexation of metal ions. The results showed that the difference between dissolution rate determined with noncomplexing buffer and that determined with traditional buffers was negligible. (3) Static tests were conducted in five buffer solutions in the pH range 4.8-9.8 at 20 C with HIP sodalite, HIP glass, and HIP CWF. The results showed that the model adequately predicts the dissolution rate of these materials at 20 C. (4) Static tests at 20 and 70 C with CWF made by the PC process indicated that the model parameters extracted from the results of tests with HIP CWF could be applied to PC CWF. (5) The dissolution rates of a modified glass made with a composition corresponding to 80 wt% glass and 20 wt% sodalite were measured at 70 C to evaluate the sensitivity of the rate to the composition of binder glass in the CWF. The dissolution rates of the modified binder glass were indistinguishable from the rates of the binder glass. (6) The dissolution rate of a simple five-component glass (CSG) was measured at 70 C using static tests and single-pass flow-through (SPFT) tests. Rates were similar for the two methods; however, the measured rates are about 10X higher than the rates measured previously at Lawrence Livermore National Laboratory (LLNL) for a glass having the same composition using an SPFT test method. Differences are attributed to effects of the solution flow rate on the glass dissolution rate and how the specific surface area of crushed glass is estimated. This comparison indicates the need to standardize the SPFT test procedure.« less
  • A ceramic waste form (CWF) of glass bonded sodalite is being developed as a waste form for the long-term immobilization of fission products and transuranic elements from the U.S. Department of Energy's activities on spent nuclear fuel conditioning. A durable waste form was prepared by hot isostatic pressing (HIP) a mixture of salt-loaded zeolite powders and glass frit. During HIP the zeolite is converted to sodalite, and the resultant CWF is been completed for durations of up to 182 days. Four dissolution modes were identified: dissolution of free salt, dissolution of the aluminosilicate matrix of sodalite and the accompanying dissolutionmore » of occluded salt, dissolution of the boroaluminosilicate matrix of the glass, and ion exchange. Synergies inherent to the CWF were identified by comparing the results of the tests with pure glass and sodalite with those of the composite CWF.« less
  • A glass-bonded sodalite ceramic waste form is being developed for the long-term immobilization of salt wastes that are generated during spent nuclear fuel conditioning activities. A durable waste form is prepared by hot isostatic pressing (HIP) a mixture of salt-loaded zeolite powders and glass frit. A mechanistic description of the corrosion processes is being developed to support qualification of the CWF for disposal. The initial set of characterization tests included two standard tests that have been used extensively to study the corrosion behavior of high level waste (HLW) glasses: the Material Characterization Center-1 (MCC-1) Test and the Product Consistency Testmore » (PCT). Direct comparison of the results of tests with the reference CWF and HLW glasses indicate that the corrosion behaviors of the CWF and HLW glasses are very similar.« less