不同晶核剂对硼硅酸盐钙钛锆石固化体析晶行为及化学稳定性的影响  

The Effects of Different Nucleation Agents on the Crystallization Behavior and Chemical Stability of the Zirconolite-based Borosilicate Glass-Ceramics

作　　者：耿安东 朱永昌 崔竹 张浩 竹含真 韩勖 霍冀川[1] GENG Andong;ZHU Yongchang;CUI Zhu;ZHANG Hao;ZHU Hanzhen;HAN Xu;HUO Jichuan(State Key Laboratory of Environmentally-Friendly Energy Materials,School of Materials Science and Engineering,Southwest University of Science and Technology,Mianyang 621900;China Building Materials Academy,Beijing 100024)

机构地区：[1]西南科技大学材料科学与工程学院环境友好能源材料国家重点实验室,绵阳621900 [2]中国建筑材料科学研究总院有限公司,北京100024

出　　处：《材料导报》2018年第22期3979-3983,3988,共6页Materials Reports

摘　　要：通过"一步法"热处理制备含24%(质量分数)模拟核废物的硼硅酸盐钙钛锆石固化体,从析晶动力学角度出发,利用Kinssinger法研究不同晶核剂(Fe_2O_3、Cr_2O_3、P_2O_5、CaF_2)作用下固化体的析晶行为及其对化学稳定性的影响。实验结果表明,Cr_2O_3的引入促进了板状CaZrTi_2O_7晶体的析出,析晶活化能E由218kJ/mol降至128kJ/mol,并使残留在玻璃基体中的模拟核素进入所析出的晶相,而其他晶核剂对析晶无明显影响。MCC-1标准测试法结果显示,Cr_2O_3作为晶核剂时,模拟核素Ce元素抗浸出性能最为优异,化学稳定性最佳,7d后归一化元素浸出率小于10^(-7) g·m^(-2)·d^(-1)。The zirconolite-based borosilicate glass-ceramics containing 24wt% simulated nuclear waste was prepared by the “one-step” thermal treatment, from the perspective of crystallization kinetics, the action of the solidified bodies’ crystallization behavior and the effect of chemical stability under different nucleation agent （Fe 2O 3, Cr 2O 3, P 2O 5, CaF 2） were investigated. As a result, the addition of Cr 2O 3 has led to the precipitation of tabular CaZrTi 2O 7 crystals and the energy E of crystallization activation decreased from 218 kJ/mol to 128 kJ/mol, and promoting the simulated nuclide remaining in the glass matrix to fuse into the precipitated crystal phase, yet other nucleation agents did not produce obvious effect. The MCC-1 experiment of glass-ceramics showed that the excellent leaching resistance and chemical stability under the impact of Cr 2O 3, and the normalized leaching rate of Ce below 10^-7 g· m^-2 ·d^-1 after 7 d.

关 键 词：玻璃陶瓷固化 钙钛锆石 化学稳定性 析晶 

分 类 号：TQ171[化学工程—玻璃工业]