Glass-ceramics with internally crystallized pyrochlore for the immobilization of uranium wastes

In this work, pyrochlore glass-ceramics (GCs)for uranium immobilization were synthesized by a pretreatment and melting-heat treatment method. The effects of different uranium contents on the phase composition, microstructure, uranium valence and chemical durability of the glass-ceramics were systematically investigated. With increasing uranium content, pyrochlore was always the dominant phase internally crystallized in the glass. CaAl2Si2O8, UTi2O6 and U3O8 were gradually observed as minor phases in the glass-ceramics. The growth of pyrochlore enriched with uranium at different uranium contents and the overall distribution of uranium in the glass-ceramics were revealed by SEM. The uranium valence states in the samples were confirmed by XPS to be a mixture of tetravalent and hexavalent states. In addition, the GC3 sample with a high uranium waste content of 16.96 wt% exhibited a low uranium leaching rate.