LnPO4·nH2O rhabdophane/monazite is an important actinide-bearing material in the back end of the nuclear fuel cycle. In this work, using Nd3+ to simulate trivalent actinides, Ce0.5Nd0.5PO4·0.667H2O rhabdophane was synthesized by the wet-chemistry method in 90 °C and pH = 1 solution. The sintering behavior of associated Ce0.5Nd0.5PO4 monazite ceramics was investigated by pressureless sintering and spark plasma sintering (SPS), along with appraising their chemical stability. The results reveal that Ce3+ is successfully replaced by Nd3+ in the rhabdophane lattice, and rhabdophane can transform to monazite with a temperature over 750 °C. SPS can compact the ceramic sample at a lower temperature compared to pressureless sintering even if the grain size is smaller. Adding a pre-sintering process of 900 °C before SPS and pressureless sintering will further improve the density and Vickers hardness of ceramics. For the chemical stability of Ce0.5Nd0.5PO4 monazite ceramics, Ce is more likely to be leached compared to Nd, and the ceramics prepared by SPS with a pre-sintering process have the lowest normalized leaching rates, associated with the values of 2.03 × 10−5 g·m−2·d−1 and 0.75 × 10−5 g·m−2·d−1 for Ce and Nd, respectively.
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