Hostname: page-component-77c89778f8-swr86 Total loading time: 0 Render date: 2024-07-17T13:54:35.439Z Has data issue: false hasContentIssue false

The Long-Term Corrosion Behavior of Titanate Ceramics for Pu Disposition: Rate-Controlling Processes

Published online by Cambridge University Press:  10 February 2011

A. J. Bakel
Affiliation:
Argonne National Laboratory, Chemical Technology Division, 9700 S. Cass Avenue, Argonne, IL60439
C. J. Mertz
Affiliation:
Argonne National Laboratory, Chemical Technology Division, 9700 S. Cass Avenue, Argonne, IL60439
M. C. Hash
Affiliation:
Argonne National Laboratory, Chemical Technology Division, 9700 S. Cass Avenue, Argonne, IL60439
D. B. Chamberlain
Affiliation:
Argonne National Laboratory, Chemical Technology Division, 9700 S. Cass Avenue, Argonne, IL60439
Get access

Abstract

The aqueous corrosion behavior of a zirconolite-rich titanate ceramic was investigated with the aim of describing the rate-controlling process or processes. This titanate ceramic is similar to SYNROC and is proposed as immobilization materials for surplus Pu. The corrosion behavior was described with results from MCC-I and PCT-B static dissolution tests. Three important observations were made: a) Ca is released at a constant rate [7×10−5 g/(m2 day)] in PCT-B tests for up to two years; b) the leachates from PCT-B tests are saturated with respect to both rutile and anatase, and c) the release rates for Pu and Gd increase with time (up to two years) in PCT-B tests. The first observation suggests that the ceramics continue to corrode at a low rate for at least 2 years in PCT-B tests. The second observation suggests that the approach to saturation with respect to these TiO2 phases does not limit the corrosion rate in PCT-B tests. The third observation suggests that the release rate of Pu and Gd are controlled by some unique process or processes, i.e., some process or processes that do not affect the release rate of other elements. While these processes cannot be fully described at this point, two possible explanations, alteration phase formation and grain boundary corrosion are forwarded.

Type
Research Article
Copyright
Copyright © Materials Research Society 2000

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1 Myers, B. R., Armantrout, G. A., Jantzen, C. M., Jostons, A., McKibben, J. M., Shaw, H. F., Strachan, D. M., and Vienna, J. D., Technical Evaluation Panel Summary Report: Ceramic and Glass Immobilization options, Lawrence Livermore National Laboratory, Livermore, CA, Report UCRL-ID-129315 (1998)Google Scholar
2 ASTM, Standard Test Method for Static Leaching of Monolithic Waste Forms for Disposal of Radioactive Waste, ASTM Standard C1220-98, American Society for Testing and Materials, Philadelphia, PA (1998).Google Scholar
3 ASTM, Standard Test Methods for Determining Chemical Durability of Nuclear Waste Glasses: The Product Consistency Test (PCT), ASTM Standard C 1285-94, American Society for Testing and Materials, Philadelphia, PA (1994).Google Scholar
4 Buck, E. C., Ebbinghaus, B. B., Bakel, A. J., and Bates, J. K., “Characterization of a Plutonium-Bearing Zirconolite-Rich Ceramic,” Mater. Res. Soc. Symp. Proc. 465, 12591266 (1997).Google Scholar
5 Bakel, A. J., Buck, E. C., Mertz, C. J., Chamberlain, D. B., and Wolf, S. F., “Corrosion Behavior of a Zirconolite-rich Ceramic”, Lawrence Livermore National Laboratory, Livermore, CA, Report PIP 99-045 (1999).Google Scholar
6 Ringwood, A. E., Oversby, V. M., Kesson, S. E., Sinclair, W., Ware, N., Hibberson, W., and Major, A., “Immobilization of High-Level Nuclear Reactor Wastes in Synroc: A Current Appraisal,” Nucl. Chem. Waste Manage. 2, 287305 (1981).Google Scholar
7 Fontana, M. G., Corrosion Engineering, 3rd ed., McGraw-Hill, New York (1986).Google Scholar
8 Smith, K. L., Colella, M., Thorogood, G. J., Blackford, M. G., Lumpkin, G. R., Hart, K. P., Prince, K., Loi, E., and Jostsons, A., “Dissolution of Synroc in Deionized Water at 150°C,” Mater. Res. Soc. Symp. Proc. 465, 349354 (1997).Google Scholar
9 Lumpkin, G. R., Smith, K. L., and Blackford, M. G., “Electron Microscope Study of Synroc Before and After Exposure to Aqueous Solutions,” J. Mater. Res. 6, 22182233 (1991).Google Scholar
10 Bourcier, W. L., “Interim Report on the Development of a Model to Predict Dissolution Behavior of the Titanate Waste Form in a Repository,” Lawrence Livermore National Laboratory, Livermore, CA, UCRL-ID-135363 (1999).Google Scholar
11 Knauss, K. G., Dibley, M. J., Bourcier, W. L., and Shaw, H. F., “Ti(IV) hydrolysis Constants Derived from Rutile Solubility Measurements made from 100°C to 300°C,” Lawrence Livermore National Laboratory, Livermore, CA, UCRL-JC-135165. (1999).Google Scholar
12 Robie, R. A., Hemingway, B. S., and Fisher, J. R., U. S. Geological Survey Bulletin 1452, U.S. Government Printing Office, Washington, DC (1979).Google Scholar
13 Lencka, M. M. and Ritman, R. E., “Thermodynamic Modeling of Hydrothermal Synthesis of Ceramic Powders,” Chem. Mater. 5, 6170 (1993).Google Scholar
14 Bakel, A. J., Ebert, W. L., and Luo, J. S., “Long-Term Performance of Glasses for Hanford Low-Level Waste”, in “Environmental Issues and Waste Management Technologies in the Ceramic and Nuclear Industries”, Ceramic Transactions, Vol. 61, Eds., Jain, V. and Palmer, R., Am. Ceram. Soc. (1995).Google Scholar