Radiation Damage of Lu2Ti2O7 and Lu2TiO5 Ceramics Caused by Kr Ion Irradiation
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摘要: 钛酸盐因其优异的物理化学性能，可作为高放射性核废物（HLW）和锕系元素（钚）的重要候选固化材料之一。采用传统的陶瓷烧结工艺制备了多晶的Lu2Ti2O7和Lu2TiO5陶瓷材料。在室温下，用800 keVKr2+对两种材料进行辐照，辐照后的样品采用GIXRD进行表征，观察到两种样品都经历了先肿胀、然后再发生非晶相变的过程。不同的是Lu2Ti2O7的晶格肿胀程度大于Lu2TiO5。另外，Lu2TiO5样品的辐照到2×1014 ions/cm2时非晶含量达95.54%，而Lu2Ti2O7样品在此剂量下非晶含量只有74.66%。通过第一性原理计算了Lu2Ti2O7晶体的晶格肿胀随反位浓度的变化关系，结果表明，Lu2Ti2O7出现非晶前的晶格肿胀主要由阳离子反位导致，而Lu2TiO5是无序的萤石结构，其辐照所导致的晶格肿胀不含阳离子反位的贡献，晶格肿胀程度较低。Abstract: Titanate are one of the important candidates for solidifying high-level radioactive nuclear waste (HLW) and lanthanide (Plutonium) due to its excellent physical and chemical durability. Polycrystalline Lu2Ti2O7 and Lu2TiO5 ceramic materials were prepared by a conventional ceramic sintering process, then the samples were irradiated with 800 keV Kr2+ at room temperature, and were subsequently characterized by GIXRD method. In the two kinds of samples, lattice swelling was observed firstly, and then amorphization phase transition took place. However, the lattice swelling of Lu2Ti2O7 is greater than that of Lu2TiO5. In addition, when Lu2Ti2O7 and Lu2TiO5 were irradiated to a fluence of 2×1014 ions/cm2, the amorphous content of Lu2TiO5 sample reaches 95.54%, while the amorphous content of Lu2Ti2O7 sample is only 74.66%. The first-principle was used to calculate the lattice swelling of Lu2Ti2O7 with increasing of anti-sites concentration. The results show that the lattice swelling of Lu2Ti2O7 before amorphization is mainly caused by the cation anti-sites. While the pristine Lu2TiO5 is a disordered fluorite structure, so that no cation anti-sites will contribute to the lattice swelling of Lu2TiO during the ion irradiation process. Therefore, the lattice swelling of Lu2TiO5 is lower compared to that of Lu2Ti2O7.
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Key words:
- irradiation /
- lattice swelling /
- amorphous phase transition /
- first-principle
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