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Durabilities of Pyrochlore-Rich Titanate Ceramics Designed for Immobilization of Surplus Plutonium

  • Y. Zhang (a1), K.P. Hart (a1), M.G. Blackford (a1), B.S. Thomas (a1), Z. Aly (a1), G.R. Lumpkin (a1), M.W. Stewart (a1), P.J. Mcglinn (a1) and A. Brownscombe (a1)...

Abstract

The chemical durabilities of two Pu-doped pyrochlore samples were studied by Single-Pass-Flow-Through (SPFT) tests at 70°C. The dissolution of pyrochlore is incongruent with preferential releases of Ca and Gd over Ti, close to stoichiometric releases of U and Ti, and lower releases of Hf and Pu than Ti. Altered pyrochlore and polymorphs of TiO2 (brookite and probably anatase) have been identified on the surface of the leached sample and the principal secondary phase is an unknown polymorph of TiO2 containing Hf and varying amounts of Gd and Pu. These surface alteration phases are consistent with reported studies of natural samples. The releases of U, Gd, Ca and Ti into solution follow linear kinetics, whereas the releases of Pu and Hf exhibit non-linear behavior. The presence of ∼5% PuO2 and trace amounts of glass does not appear to have an effect on the overall durability of the material. Further, the low Pu release rate and the similar kinetics for Pu and Hf releases limit the possibility of nuclear criticality under repository conditions. Overall, this study provides useful information on the lower bounds of durabilities of the materials.

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References

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Durabilities of Pyrochlore-Rich Titanate Ceramics Designed for Immobilization of Surplus Plutonium

  • Y. Zhang (a1), K.P. Hart (a1), M.G. Blackford (a1), B.S. Thomas (a1), Z. Aly (a1), G.R. Lumpkin (a1), M.W. Stewart (a1), P.J. Mcglinn (a1) and A. Brownscombe (a1)...

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