Nd-doped ZrSiO4 Ceramics: Synthesis in Molten Salt at Low Temperature, Phase Evolution and Chemical Stability

In contrast to conventional solid-phase sintering, molten salt method can provide a fast mass transfer and nucleation process at lower temperatures which has potential to synthesize the ceramic solid solution for immobilization of high-level nuclear waste (HLW). In this work, Nd-doped zircon (ZrSiO4) ceramics (Zr1-xNdxSiO4-x/2 (0 <= x <= 0.1)) were prepared by the molten salt synthesis(MSS) at different sintering temperatures (1100, 1200, 1300, 1400, 1500 degrees C) for different sintering time (3, 6, 9, 12, and 15 h). Chemical stability of Nd-doped zircon ceramics in simulated geological disposal environment was studied by static leaching test (PCT). Zr1-xNdxSiO4-x/2 was synthesized by the molten salt method under the optimum molar ratio of molten salt to oxide at 10:1, sintering temperature at 1200 degrees C and sintering time of 6 h with the solid solution of Nd in ZrSiO4 being increased to 8% (in mol). The MSS can reduce the synthetic temperature, shorten the sintering time and save the solid solution. The immobilizing mechanism of ZrSiO4 ceramics for trivalent actinide nuclides is lattice immobilizing. Experimental results show that the normalized leaching rate (LRNd) of Nd is as low as similar to 10(-5) g center dot m(-2)center dot d(-1). ZrSiO4 ceramics have no phase evolution before and after leaching, suggesting good structural stability. TLeaching model consolidates that Nd leaching is due to dissolution of the ceramic surface layer. Data from this study show that MSS is a promising method to synthesize ceramics solid solution.