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Evaluation of Standard Durability Tests Towards the Qualification Process for the Glass-Zeolite Ceramic Waste Form

Published online by Cambridge University Press:  03 September 2012

L. J. Simpson  and
D. J. Wronkiewicz
L. J. Simpson
Affiliation:
Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439
D. J. Wronkiewicz
Affiliation:
Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439
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Abstract

Glass-bonded zeolite is being developed as a potential ceramic waste form for the disposition of radionuclides associated with the U.S. Department of Energy's (DOE's) spent nuclear fuel conditioning activities. The utility of several standard durability tests [e.g., Materials Characterization Center Test #1 (MCC-1), Product Consistency Test-B (PCT-B), and Vapor Hydration Test (VHT)] was evaluated as a first step in developing methods and criteria that can be applied towards the process of qualifying this material for acceptance into the DOE Civilian Radioactive Waste Management System. The effects of pH, leachant composition, and sample surface-area-to-leachant-volume ratios on the durability test results are discussed, in an attempt to investigate the release mechanisms and other physical and chemical parameters that are important for the acceptance criteria, including the establishment of appropriate test methodologies required for product consistency measurements.

Results from PCT-Bs conducted with 4 μm diameter salt-loaded zeolite powder indicate that a good correlation exists between release rate and ionic size and/or charge for the release behavior of the simulated fission products in deionized water (DRV), EJ-13 groundwater, and brine solutions. Simulated divalent and trivalent fission products [Sr, Ba, and rare earth (RE) ions] were preferentially retained in the zeolite (relative to the singly ionized cations) after tests with the salt-loaded zeolite in DIW. In general, the preferential cation release order for salt-loaded zeolite A in DrW is Li > Na ≥ K > Cs > Al > Si > RE > Sr > Ba. Results from PCT-Bs with the salt-loaded zeolite A immersed in high-ionic-strength brines at 90°C indicate a significant increase, relative to DIW tests, in the release rates of the Sr, Ba, and RE ions despite a decrease in the release of the Si and Al ions that make up the framework matrix of the zeolite. An increase in the Mg and Ca concentrations in the reacted zeolites suggests that an ion exchange process may be responsible for this increase.

Vapor hydration and MCC-1 tests were performed with ceramic waste form monoliths of glass-bonded zeolite. The VHTs (temperatures at 120,150, and 200°C) provided useful information about the effect of glass composition on corrosion rates and alteration phase formation, and about the overall toughness and structural integrity of the ceramic waste form. The MCC-1 test was investigated as an alternative to the PCT for acceptance criteria measurements. The MCC-1 results indicate that corrosion testing with both DIW and high-ionic-strength leachants (that specifically affect the ion exchange behavior of the fission products) are required to fully assess the durability of the ceramic waste form. These preliminary results establish the utility of the MCC-1 test for providing possible acceptance criteria measurements, including elemental release comparisons between the environmental assessment benchmark and the ceramic waste form.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 465: Symposium II – Scienfific Basis for Nuclear Waste Management XX , 1996 , 441
Copyright
Copyright © Materials Research Society 1997

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References

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