Abstract

AbstractTwo ceramics for immobilization of a Zr-REE-actinide fraction of high level waste (HLW) based on zirconolite or/and pyrochlore structures with minor brannerite/lucasite, and fluorite-structured dioxide-based solid solution, were synthesized and characterized. The samples were produced by melting of oxide mixtures at 1500 °C followed by controlled cooling for crystallization. Phase compositions of the samples obtained and waste elements partitioning among co-existing phases were investigated in detail using powder X-ray diffraction, scanning electron microscopy with energy dispersive spectroscopy, and transmission electron microscopy. Cerium enters cerianite-based solid solution, lucasite (if present), and to a lesser extent, pyrochlore and zirconolite. Europium and gadolinium enter predominantly zirconolite and pyrochlore. The highest uranium concentrations were found in a uraninite-based cubic solid solution or pyrochlore and zirconolite.

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