• Nuclear Engineering and Technology
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• v.54 no.7
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• pp.2427-2434
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• 2022

Series of unequal quantity Nd/Ce co-doped ceramic nuclear waste forms, (Gd, Nd)₂(Zr, Ce)₂O₇, were prepared to tailor its ordered pyrochlore or disordered fluorite structure. The phase transition, microtopography, and elemental composition of the ceramic samples were systematically investigated, especially the effect of order-disorder structure on the chemical stability. It was confirmed that unequal quantity of Nd/Ce could synchronously replace the Gd/Zr-sites of Gd₂Zr₂O₇. And the phase transition of order-disorder structure could be successfully tailored by regulating the average cationic radius ratio of (Gd, Nd)₂(Zr, Ce)₂O₇ series. The elements of Gd, Nd, Zr, and Ce are uniformly distributed in the ordered or disordered structures. The MCC-1 leaching results showed that (Gd, Nd)₂(Zr, Ce)₂O₇ pyrochlore ceramic nuclear waste forms had excellent chemical stability, whose elements' normalized leaching rates were as low as 10^-4-10^-7 g·m^-2·d^-1 after 7 days. In particular, the chemical stability of disordered structure was superior to that of ordered structure. It was proposed that the force constant and the closest packing were changed with the structure transformation resulting the chemical stability difference.