氧化镨对高钠硼硅酸盐废物玻璃结构的作用及化学性能的影响

Effect of Praseodymium Oxide on Glass Structure and Chemical Propertiesof High Sodium Borosilicate Waste

  • 摘要: 随着反应堆乏燃料燃耗的升高,高放废液中镧系和锕系元素含量增多。本文针对高燃耗乏燃料高放废液中含量较高的氧化镨对高钠硼硅酸盐玻璃结构和性能的影响进行研究。结果显示,在废物包容量10wt.%条件下,氧化镨添加量10wt.%的玻璃样品仍可维持均匀的玻璃无定形结构。拉曼分析结果显示,随着氧化镨的添加,1 065 cm−1附近的峰有向左偏移的趋势,玻璃结构Q3占比出现减少趋势。29Si固态核磁分析结果显示,随着废物添加量的增加和氧化镨的加入,Q4和Q3占比呈先减少后增加的趋势,同时Q2和Q1占比呈先增加后减少的趋势,表明废物添加量的增加和氧化镨的加入使得玻璃网络结构聚集度呈先降低后提高,氧化镨主要充当网络结构调节剂。化学稳定性测试结果显示,在废物包容量0wt.%条件下,随着氧化镨的加入,元素浸出率升高;在废物包容量10wt.%条件下,随着氧化镨的加入,元素浸出率逐步下降。表明废物包容量的增加和氧化镨的添加能够促进玻璃网络结构趋于聚集和稳定化,提高化学稳定性。

     

    Abstract: With the increase of spent fuel burnup, the lanthanide and actinide elements in high-level radioactive waste liquid increase. This article focuses on the influence of praseodymium oxide, which has a high content in high-level radioactive waste liquid of spent fuel burnup, on the structure and properties of high sodium borosilicate glass. The research results show that when the waste capacity is 10wt.% and the amount of praseodymium oxide added is 10wt.%, the glass sample can still maintain a uniform amorphous glass structure. The Raman analysis results show that with the addition of praseodymium oxide, the peak near 1 065 cm−1 tends to shift to the left, and the glass structure Q3 exhibits decreasing trend. The nuclear magnetic resonance analysis results show that with the increase of waste addition and the addition of praseodymium oxide, Q4 and Q3 show a trend of firstly decreasing and then increasing, while Q2 and Q1 show a trend of firstly increasing and then decreasing, indicating that the increase in the addition of waste and praseodymium oxide causes the aggregation degree of the glass network structure to firstly decrease and then increase. The chemical stability test results show that under the condition of a waste loading of 0wt.%, the leaching rate of the element increases with the addition of praseodymium oxide. Under the condition of a waste loading of 10wt.%, the leaching rate decreases with the addition of praseodymium oxide, suggestting as the waste loading increases, the glass network structure tends to aggregate and stabilize with the praseodymium oxide addition.

     

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