YIG陶瓷对三价锕系模拟核素的固化行为研究

石榴石具有较大的锕系包容量及化学灵活性, 被认为是潜在的锕系核素固化基材。本工作以Nd³⁺模拟三价锕系核素, 通过高温固相法成功合成了Y_3-xNd_xFe₅O₁₂(0≤x≤2)系列钇铁石榴石(YIG)固化体。研究了Nd在YIG固化体中的固溶极限和Nd掺杂量对固化体的物相和微观结构的影响规律, 以及不同pH条件下Nd掺杂钇铁石榴石固化体的化学耐久性。研究结果表明, 当x≤1.7时, YIG基固化体为纯相YIG; 当x≥1.8时, YIG基固化体中YIG、NdFeO₃和Fe₂O₃三相共存。纯相YIG基固化体对Nd³⁺的固溶极限约为29.5%(质量分数)。随着Nd掺杂量增加, 固化体的密度增大, 体积减小, 孔隙率减小。浸出实验结果显示, 28 d后元素归一化浸出率(LR_i)逐渐趋于平衡, 42 d后, 其元素的LR_i为10^-6~10^-5 g·m^-2·d^-1。LR_Y小于LR_Nd, 且酸性溶液中元素归一化浸出率也略高于中性和碱性溶液。这些结果表明, YIG陶瓷是理想的三价锕系核素候选固化基材。

Immobilizing Behavior of Trivalent Actinide Nuclides by YIG Ceramics

Garnet is considered as a potential matrix for immobilizing high-level radioactive waste (HLW) because of its large actinide package capacity and chemical flexibility. Y_3-xNd_xFe₅O₁₂ (0≤x≤2) series yttrium iron garnet (YIG) samples was successfully synthesized by solid-state sintering method using Nd³⁺ to simulate trivalent actinides. The solubility limit of Nd in the YIG and the influence of Nd doping amount on the phase and microstructure of ceramics was studied. Then the chemical durability of Nd-doped yttrium iron garnet solidified body under different pH conditions was evaluated. The results show that the ceramics with x≤1.7 show homogeneous single YIG, but the ceramics with x≥1.8 exhibit coexistence of three crystal phases (YIG, NdFeO₃ and Fe₂O₃). The solubility limit of Nd³⁺ in the pure YIG is about 29.5% (in mass). As the amount of Nd doping increases, the density of the ceramics increases, the volume decreases, and the porosity decreases. The leaching experiment results show that the normalized leaching rate of the elements (LR_i) is 10^-6~10^-5g·m^-2·d^-1. LR_Y is smaller than LR_Nd, and the normalized leaching rate of the elements in acid leachate is slightly higher than those in neutral and alkaline leachates. The results indicate that YIG ceramics are a potential candidate form for trivalent actinides.