Nd2O3对钼酸钙-钙钛锆石硼硅酸盐玻璃陶瓷结构和性能的影响  

Effect of Nd_(2)O_(3) on Structure and Properties of Powellite-Zirconolite Borosilicate Glass Ceramics

作　　者：连启会 张行泉 霍冀川 吴浪[1] 张壮森 LIAN Qihui;ZHANG Xingquan;HUO Jichuan;WU Lang;ZHANG Zhuangsen(School of Materials Science and Engineering,Southwest University of Science and Technology,Mianyang 621010,Sichuan,China;Analytical and Testing Center,Southwest University of Science and Technology,Mianyang 621010,Sichuan,China)

机构地区：[1]西南科技大学材料科学与工程学院,四川绵阳621010 [2]西南科技大学分析测试中心,四川绵阳621010

出　　处：《材料导报》2022年第7期163-167,共5页Materials Reports

基　　金：国家自然科学基金(11775182)。

摘　　要：针对乏燃料后处理产生的高放废液中具有镧系元素(Ln)和过渡金属元素(Mo)含量较高的特点,本实验开发了一种以钼酸钙和钙钛锆石为主晶相的硼硅酸盐玻璃陶瓷固化体,并研究了Nd_(2)O_(3)含量(0%~5%,摩尔分数,下同)对玻璃陶瓷固化体的物相组成、形貌结构和抗浸出性能的影响。结果表明,Nd_(2)O_(3)含量为0%~3%的固化体仅含均匀分布在玻璃基质中的钼酸钙和钙钛锆石两种晶相;随Nd_(2)O_(3)含量增加,固化体的BO_(4)向BO_(3)转变,玻璃陶瓷固化体的体积密度和氧堆积密度逐渐增加,结构变得更加致密;产品一致性测试(PCT)结果表明,28 d后含Nd_(2)O_(3)玻璃陶瓷的Mo浸出率相较于不含Nd_(2)O_(3)玻璃陶瓷的Mo浸出率(LR)低了约两个数量级,其中Nd_(2)O_(3)含量为3%样品的LR_(Si)、LR_(Ca)、LR_(Mo)和LR_(Nd)分别约为1.90×10^(-3)g·m^(-2)·d^(-1)、6.38×10^(-4)g·m^(-2)·d^(-1)、8.27×10^(-5)g·m^(-2)·d^(-1)和1.42×10^(-6)g·m^(-2)·d^(-1)。In this paper,a borosilicate glass-ceramic waste form with powellite and zirconolite as the main crystalline phases was developed,for the high content of lanthanide(Ln)and transition metal(Mo)in high-level liquid waste arising from spent nuclear fuel reprocessing,and the phase composition,structure and leaching properties of glass-ceramic forms with content of 0 mol%—5 mol%Nd_(2)O_(3)were investigated.The results show that two major target phases,powellite and zirconolite,are observed for the glass-ceramics with 0 mol%—3 mol%Nd_(2)O_(3),which are homogenously distributed in the glass matrix.With Nd_(2)O_(3)addition,the BO_(4)group transformed to BO_(3),bulk density and oxygen packing density gra-dually increased,and the structure became denser.PCT result shows that after 28 d,the leaching rate of glass-ceramic incorporated Nd_(2)O_(3)reduced by about two orders of magnitude lower than that of those without Nd_(2)O_(3)glass ceramic,and for the sample with 3 mol%Nd_(2)O_(3),of which LR;,LR;,LR;and LR;are approximately 1.90×10^(3)g·m^(-2)·d^(-1),6.38×10^(4)g·m^(-2)·d^(-1),8.27×10^(5)g·m^(-2)·d^(-1)and 1.42×10^(6)g·m^(-2)·d^(-1).

关 键 词：高放废液 玻璃陶瓷 钼酸钙 钙钛锆石 抗浸出性能 

分 类 号：TL24[核科学技术—核燃料循环与材料] TQ171.733[化学工程—玻璃工业]