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Title:
Uranium release and secondary phase formation during unsaturated testing of UO2 at 90°C
Authors:
Wronkiewicz, David J.; Bates, John K.; Gerding, Thomas J.; Veleckis, Ewald; Tani, Benjamin S.
Affiliation:
Argonne National Laboratory, Chemical Technology Division, 9700 South Cass Avenue, Argonne, IL 60439-4837,USA
Publication:
Journal of Nuclear Materials, Volume 190, p. 107-127.
Publication Date:
08/1992
Origin:
ELSEVIER
Abstract Copyright:
Elsevier Science Publishers B.V. All rights reserved.
DOI:
10.1016/0022-3115(92)90081-U
Bibliographic Code:
1992JNuM..190..107W

Abstract

Experimental results indicate that UO2 will readily react after being exposed to dripping oxygenated ground water at 90°C. A pulse of rapid U release, combined with the formation of dehydrated schoepite characterizes reactions between one to two years. Rapid dissolution of intergrain boundaries and spallation of UO2 granules appears to be responsible for the rapid U release. Less than 5% of the U is released in a soluble or suspended form. After two years, U release rates decline and a more stable assemblage of uranyl silicate phases form by incorporating cations from the leachant. Uranophane, boltwoodite, and sklodowskite are the final solubility-limiting phases for U in these tests. This observed paragenetic sequence (from uraninite to schoepite to uranyl silicates) is identical to those observed in weathered uraninite deposits. Dispersion of particulate matter may be an important release mechanism for U and other radionuclides in spent nuclear fuel.
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