Hostname: page-component-586b7cd67f-dsjbd Total loading time: 0 Render date: 2024-11-28T08:40:51.512Z Has data issue: false hasContentIssue false

Can Spent Nuclear Fuel Decay Heat Prevent Radionuclide Release?

Published online by Cambridge University Press:  17 March 2011

James L. Jerden Jr.
Affiliation:
Argonne National Laboratory, Argonne, IL, USA
Margaret M. Goldberg
Affiliation:
Argonne National Laboratory, Argonne, IL, USA
James C. Cunnane
Affiliation:
Argonne National Laboratory, Argonne, IL, USA
Theodore H. Bauer
Affiliation:
Argonne National Laboratory, Argonne, IL, USA
Roald A. Wigeland
Affiliation:
Argonne National Laboratory, Argonne, IL, USA
Russell E. Nietert
Affiliation:
Argonne National Laboratory, Argonne, IL, USA
Get access

Abstract

Heat generated by radioactive decay of spent fuel represents a potentially important barrier to water accumulation on commercial spent nuclear fuel in breached waste packages. In the absence of water, fuel degradation and radionuclide release will be negligible. Thermal models for the proposed Yucca Mountain Repository suggest that, after a period of approximately 1000-4000 years (depending on loadingand ventilation conditions), the repository drift walls may decline to sub-boiling temperatures, thus allowing humidity in the drift to increase. The question thus arises, is the thermal gradient between the fuel and the drift sufficient to prevent water accumulation in a humid drift environment throughout the regulatory period? The answer depends on the balance between processes that oppose water condensation ontothe fuel (decay heat) and those that promote condensation such as the deliquescence of hygroscopic phaseswithin the fuel.

Our experimental results indicate that deliquescence could lead to the condensation of water onto spent fuel despite the thermal “self-drying”effect if the following criteria are met: (1) the fission product salt CsI is present in the fuel or in the fuel-cladding gap, (2) the relative humidity in the driftexceeds 80% while temperatures in the waste package are around 90oC. Previous work suggests that these criteria may be met for some fuel pins within the proposed Yucca Mountain Repository. However,experiments that account for the role of U(VI) alteration phases suggest that deliquescence may be a self-limiting process in the sense that deliquescent components (e.g. Cs, Ba, Sr) may be incorporatedinto nondeliquescent U(VI) phases that form from the corrosion of spent fuel.

Type
Research Article
Copyright
Copyright © Materials Research Society 2004

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

1. Cubicciotti, D., and Sanecki, J.E., Journal of Nuclear Materials, 78, 96111, (1978).Google Scholar
2. Moriyama, K, and Furuya, H., Journal of Nuclear Science and Technology, 34(9), 900908, (1997).Google Scholar
3. Goldberg, M. M., Bauer, T. H., Nietert, R. E., Wigeland, R. A., Cunnane, J. C., and Jerden, J., Spent fuel decay heat as a barrier to aqueous corrosionand radionuclide release, Annual Report: Office of Civilian Radioactive Waste Management, Science and Technology Program, October, 2003.Google Scholar
4. Plummer, L. N., Parkhurst, D. L., , Fleming, Dunkle, S. A., 1988, PHRQPITZ: A computer program incorporating Pitzer's equations for calculation of geochemical reactions in brines,U.S. Geological Survey Water-Resources Investigations Report 88–4153, 310 p.Google Scholar
5. Acheson, D. T., in Humidity and Moisture, edited by Wexler, A. and Wildhack, W. A. (Reinhold Publishing Corporation, New York, 1965), pp.521-530.Google Scholar
6. Finch, R. J. and Murakami, T., inUranium Mineralogy, Geochemistry and the Environment, Reviews in Mineralogy Volume 38, edited by Burns, P. and Finch R., (Mineralogical Society of America, Washington DC, 1999) pp. 91-179.Google Scholar
7. Fortner, J. A., Finch, R. J., Kropf, J., and Cunnane, J. C., Re-evaluating neptunium in uranyl phases derived from corroded spent fuel, accepted for publication, Nuclear Technology (2004).Google Scholar