Temperature dependences of phase composition, densification, and thermal/chemical stability of Sr0.5Zr2(PO4)3-Nd0.5Sm0.5PO4 composite ceramics for nuclear waste form

Abstract

A kind of Sr0.5Zr2(PO4)3-Nd0.5Sm0.5PO4 (hereinafter SrZP-Nd0.5Sm0.5PO4) composite ceramics was prepared through a one-step microwave sintering technique, where Sr, Nd, Sm were simulated for fission products and minor actinides (MA). The crystal structure and morphology of constituent phases were systematically characterized by XRD, TEM, and SEM techniques. The temperature dependent phase analysis results of SrZP-Nd0.5Sm0.5PO4 composite ceramics illustrate that with evaluating temperature monazite structure formed primarily, and the SrZP phase formed subsequently. With the temperature rising further, the monazite phase finally transformed into Nd0.5Sm0.5PO4 monazite solid solution. XRD refinement and TEM measurements are used to verify the crystal structures of the as-prepared SrZP and Nd0.5Sm0.5PO4 phases in the composite ceramics. The dependence of densification behaviors on temperature shows that the distinct densification of the SrZP-Nd0.5Sm0.5PO4 composite ceramics occurs in the temperature range of 950 °C to 1000 °C, and the relative density reaches 97.7 % at 1050 °C. TG-DSC tests show that the SrZP-Nd0.5Sm0.5PO4 composite ceramics exhibit excellent thermal stability at high temperatures. And SrZP-Nd0.5Sm0.5PO4 composite ceramics possess outstanding chemical stability, whose normalized leaching rate of Sr, Nd, and Sm is 10−4 g·m−2·d−1, 10−7 g·m−2·d−1, and 10−7 g·m−2·d−1 order of magnitude, respectively.