模拟锕系核素和硫在钡硼硅酸盐玻璃陶瓷固化体中的赋存状态研究

项目名称： 模拟锕系核素和硫在钡硼硅酸盐玻璃陶瓷固化体中的赋存状态研究

项目编号： No.11305135

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 数理科学和化学

项目作者： 吴浪

作者单位： 西南科技大学

项目金额： 25万元

中文摘要： 针对目前高放废液硼硅酸盐玻璃固化体存在锕系核素溶解度较低、稳定性较差等不足，以及在玻璃熔制过程中产生分离的含硫黄色第二相（黄相）问题，本项目拟采用熔融-热处理工艺制备含钙钛锆石、榍石和重晶石晶相的钡硼硅酸盐玻璃陶瓷固化体，其中钙钛锆石和榍石相用来固定模拟锕系核素（Nd、Ce），重晶石相用来固定硫元素。系统研究钡硼硅酸盐玻璃陶瓷固化体的组分和热处理工艺与晶相组成、显微结构和物理性能之间关系，探讨钙钛锆石和榍石在钡硼硅酸盐玻璃中的析晶机制，优化集成固化体的制备工艺技术；揭示模拟锕系核素（Nd、Ce）及硫元素在钡硼硅酸盐玻璃陶瓷固化体中的赋存状态，评价固化体的化学稳定性。相关研究成果可为优化和制备高性能含硫锕系高放废液玻璃陶瓷固化体提供理论依据和技术支持，为推进高放废液玻璃陶瓷固化的应用基础研究及其安全处置奠定基础。

中文关键词： 锕系核素；硫；玻璃陶瓷；钙钛锆石；重晶石

英文摘要： The borosilicate glass waste forms for the immobilization of high level liquid waste (HLLW) have some drawbacks such as the low solubility of actinides and poor thermal stability and chemical durability. In addition, a separate yellow phase containing sulfur is usually formed during the vitrification process. In this project, barium borosilicate glass-ceramic waste forms containing zirconolite, titanite, and barite crystalline phases will be prepared by melt-heat treatment technique. It is expected that the simulated actinides (Nd and Ce) are immobilized in the zirconolite and titanite phases, while the sulfur is immobilized in the barite phase. The relationships among the composition, heat treatment processing, phase structure, microstructure, and physical properties of the glass-ceramic waste forms will be studied. The crystallization mechanism of the zirconolite and titanite phases in the barium borosilicate glass will also be discussed. The processing techniques of the barium borosilicate glass-ceramic waste forms will be optimized. Furthermore, the occurrence of simulated actinides (Nd and Ce) and sulfur in the barium borosilicate glass-ceramic waste forms will be investigated. Moreover, the chemical durability of the barium borosilicate glass-ceramic waste forms will be evaluated. It is expected that the r

英文关键词： actinides；sulfur；glass-ceramics；zirconolite；barite