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用于核废料固化的碱硼硅酸盐玻璃初始浸出特性评估

An Assessment of Initial Leaching Characteristics of Alkali-Borosilicate Glasses for Nuclear Waste Immobilization.

作者信息

Farid Osama M, Ojovan M I, Massoud A, Rahman R O Abdel

机构信息

Reactors Department, Nuclear Research Center, Atomic Energy Authority of Egypt, Cairo 13759, Egypt.

Department of Materials Science and Engineering, The University of Sheffield, S1 3JD Sheffield, UK.

出版信息

Materials (Basel). 2019 May 6;12(9):1462. doi: 10.3390/ma12091462.

Abstract

Initial leaching characteristics of simulated nuclear waste immobilized in three alkali- borosilicate glasses (ABS-waste) were studied. The effects of matrix composition on the containment performance and degradation resistance measures were evaluated. Normalized release rates are in conformance with data reported in the literature. High Li and Mg loadings lead to the highest initial de-polymerization of sample ABS-waste (17) and contributed to its thermodynamic instability. Ca stabilizes non-bridging oxygen (NBO) and reduces the thermodynamic instability of the modified matrix. An exponential temporal change in the alteration thickness was noted for samples ABS-waste (17) and Modified Alkali-Borosilicate (MABS)-waste (20), whereas a linear temporal change was noted for sample ABS-waste (25). Leaching processes that contribute to the fractional release of all studied elements within the initial stage of glass corrosion were quantified and the main controlling leach process for each element was identified. As the waste loading increases, the contribution of the dissolution process to the overall fractional release of structural elements decreases by 43.44, 5.05, 38.07, and 52.99% for Si, B, Na, and Li respectively, and the presence of modifiers reduces this contribution for all the studied metalloids. The dissolution process plays an important role in controlling the release of Li and Cs, and this role is reduced by increasing the waste loading.

摘要

研究了固定在三种碱硼硅酸盐玻璃(ABS废物)中的模拟核废料的初始浸出特性。评估了基体组成对包容性能和抗降解措施的影响。归一化释放率与文献报道的数据一致。高锂和镁负载导致样品ABS废物(17)的初始解聚程度最高,并导致其热力学不稳定性。钙使非桥氧(NBO)稳定,并降低了改性基体的热力学不稳定性。样品ABS废物(17)和改性碱硼硅酸盐(MABS)废物(20)的蚀变厚度呈现指数时间变化,而样品ABS废物(25)的蚀变厚度呈现线性时间变化。对玻璃腐蚀初始阶段所有研究元素的分数释放所涉及的浸出过程进行了量化,并确定了每种元素的主要控制浸出过程。随着废物负载量的增加,溶解过程对结构元素总分数释放的贡献分别降低,硅、硼、钠和锂的降低幅度分别为43.44%、5.05%、38.07%和52.99%,并且改性剂的存在降低了所有研究类金属元素的这种贡献。溶解过程在控制锂和铯的释放方面起着重要作用,并且这种作用随着废物负载量的增加而减弱。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cf25/6539539/ac75362dbd34/materials-12-01462-g001.jpg

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