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

  • J. P. Icenhower (a1), B. P. McGrail (a1), D. M. Strachan (a1), R. D. Scheele (a1), V. L. Legore (a1), E. A. Rodriguez (a1), J. L. Steele (a1), C. F. Brown (a1) and M. J. O'Hara (a1)...

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.

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

  • J. P. Icenhower (a1), B. P. McGrail (a1), D. M. Strachan (a1), R. D. Scheele (a1), V. L. Legore (a1), E. A. Rodriguez (a1), J. L. Steele (a1), C. F. Brown (a1) and M. J. O'Hara (a1)...

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