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Experimental Determination of the Dissolution Kinetics of Plutonium- and Uranium-Bearing Ceramics at 90°C

Published online by Cambridge University Press:  21 March 2011

J. P. Icenhower ,
B. P. McGrail ,
D. M. Strachan ,
R. D. Scheele ,
V. L. Legore ,
E. A. Rodriguez ,
J. L. Steele ,
C. F. Brown  and
M. J. O'Hara
J. P. Icenhower
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
B. P. McGrail
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
D. M. Strachan
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
R. D. Scheele
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
V. L. Legore
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
E. A. Rodriguez
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
J. L. Steele
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
C. F. Brown
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
M. J. O'Hara
Affiliation:
Pacific Northwest National Laboratory, Richland, WA 99352, U.S.A.
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Abstract

As a first step toward understanding the effects of radiation damage on element release rates from Ti-bearing waste forms, we performed single-pass flow-through (SPFT) experiments with 239Pu- and 238U-bearing ceramics over a solution pH-interval of 2 to 10 at 90°C. The ceramics tested are chemically complex and are dominated volumetrically by betafite (Ti-pyrochlore) (ABTi2O7) (A = Ca2+, Gd3+, B = Gd3+, Hf4+, Pu4+, U4/6+). The 239Pu-bearing specimens contained 11.9 mass% PuO2 and 23.7 mass% UO2. In addition, a 238Pu-bearing (11.8 and 23.9 mass% PuO2 and UO2, respectively) specimen was tested at pH = 2, 90°C. The 239Pu-bearing specimens slowly released Pu to solution (rate = 7.6x10-6 g m-2 d-1), even at pH = 2. Release of elements across the pH interval investigated exhibits a weak amphoteric behavior. Compared to results from the 239Pu-bearing materials, the 238Pu-bearing specimen released Pu >1000X faster (rate = 9.3x10-3 g m-2 d-1) at pH = 2. Release rates of U, Gd, and Hf are also faster from the 238Pu-bearing ceramic compared to the specimen containing 239Pu. Although preliminary, the data can be interpreted to indicate that accumulation of radiation damage may result in faster release of Pu and U to solution than previously suspected.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 713: Symposium JJ – Scientific Basis for Nuclear Waste Management XXV , 2002 , JJ11.38
Copyright
Copyright © Materials Research Society 2002

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References

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