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Dissolution kinetics of pyrochlore ceramics for the disposition of plutonium
-
Jonathan P. Icenhower
,
B. Pete Mcgrail
Published/Copyright:
March 31, 2015
Abstract
Single-pass β ow-through (SPFT) experiments were conducted on a set of non-radioactive Ti-based ceramics at 90 °C and pH = 2 to 12. The specimens contained 27.9 to 35.8 wt%CeO2 as a surrogate for UO2 and PuO2. Compositions were formulated as TiO2-saturated pyrochlore (CeP1) and pyrochlorerich baseline (CePB1) ceramic waste forms. Pyrochlore + Hf-rutile and pyrochlore + perovskite + Hf-rutile constituted the major phases in the CeP1 and CePB1 ceramics, respectively. Results from dissolution experiments between pH = 2 to 12 indicate a shallow pH-dependence with an ill-defined minimum. Element release rates determined from experiments over a range of sample surface areas (S) and β ow rates (q) indicate that dissolution rates become independent of q/S values at 10.8 to 10.7 m/s. Dissolution rates dropped sharply at lower values of q/S, indicating rates that are subject to solution saturation effects as dissolved constituents become concentrated. Forward dissolution rates were 1.3(0.30) x 10-3 and 5.5(1.3) x 10-3 g/m2·d for CeP1 and CePB1 ceramics, respectively. Dissolution rates obtained in other laboratories compare well to the findings of this study, once the rate data are placed in the context of solution saturation state. These results make progress toward an evaluation of CeO2 as a surrogate for UO2 and PuO2 as well as establishing a baseline for comparison with radiation- damaged specimens.
Keywords : Crystal structure; radiation damage; kinetics; dissolution rate; phase transition; amorphization; XRD data
Received: 2004-5-11
Accepted: 2005-6-3
Published Online: 2015-3-31
Published in Print: 2006-1-1
© 2015 by Walter de Gruyter Berlin/Boston
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Keywords for this article
Crystal structure;
radiation damage;
kinetics;
dissolution rate;
phase transition;
amorphization;
XRD data
Articles in the same Issue
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- An FTIR study of hydrogen in anorthoclase and associated melt inclusions
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