Gamma irradiation-induced defects in borosilicate glasses for high-level radioactive waste immobilisation
Gamma irradiation-induced defects in borosilicate glasses for high-level radioactive waste immobilisation
复制标题
DOI：
10.1016/j.jnucmat.2020.152702
复制
发表时间：
2021-02
影响因子：
3.1
通讯作者：
P. Rautiyal;G. Gupta;R. Edge;L. Leay;A. Daubney;M. Patel;A. H. Jones;P. Bingham
中科院分区：
文献类型：
--
作者：
P. Rautiyal;G. Gupta;R. Edge;L. Leay;A. Daubney;M. Patel;A. H. Jones;P. Bingham
在英国和印度分别用于高放射性废物固定的硼硅酸锂钠（LiNaBSi）和硼硅酸钠钡（NaBaBSi）玻璃中，研究了剂量为0.5和5 MGy的伽马辐照引起的缺陷。用X-波段电子顺磁共振（EPR）、拉曼和紫外-可见-近红外（UV-Vis-nIR）光谱对玻璃在辐照前后进行了表征。EPR和UV-Vis-nIR吸收光谱显示，形成的硼氧空穴中心（BOHC），电子捕获在碱金属阳离子或ET中心和过氧自由基（PORs）的缺陷共同的两种玻璃。此外，在NaBaBSi玻璃中观察到E-或极化子中心，可能与元素钠胶体的形成有关。在一定温度范围内进行了随时间变化的热退火，包括与罐中心线冷却有关的温度，这可能与今后技术评估中的地质处置有关，以研究这些辐射引起的缺陷的热稳定性。据观察，PORs是两种玻璃中最热稳定的缺陷。讨论了玻璃成分对钠偏析的影响以及辐照后可能形成的金属胶体。
Gamma irradiation-induced defects at doses of 0.5 and 5 MGy were studied in lithium sodium-borosilicate (LiNaBSi) and sodium barium-borosilicate (NaBaBSi) glasses, used for high-level radioactive waste immobilisation in the UK and India, respectively. X-band electron paramagnetic resonance (EPR), Raman and UV-Vis-nIR spectroscopies were used to characterise the glasses before and after irradiation. EPR and UV-Vis-nIR absorption spectroscopies revealed the formation of boron-oxygen hole centres (BOHC), electrons trapped at alkali cations or ET centres and peroxy-radicals (PORs) as defects common to both glasses. In addition, E−or polaron centres were observed in NaBaBSi glasses, possibly related to formation of elemental sodium colloids. Time-dependent thermal annealing at a range of temperatures, including those relevant to canister centreline cooling (CCC), which may be of relevance to geological disposal in future technical assessments, was carried out to study thermal stability of these radiation-induced defects. It was observed that PORs are the most thermally-stable defects in both glasses. The influence of glass composition on the segregation of sodium and the possible formation of metal colloids upon irradiation have been discussed.