硅酸盐通报2024,Vol.43Issue(9) :3399-3406.

高熵烧绿石(La1/6 Pr1/6 Nd1/6 Sm1/6 Eu1/6 Gd1/6)2 Zr2O7固化锕系核素的结构和化学稳定性研究

Structure and Chemical Durability of Actinide Nuclides Solidified by High-Entropy Pyrochlore(La1/6Pr1/6Nd1/6Sm1/6Eu1/6Gd1/6)2Zr2O7

杜瞻远 朱永昌 崔竹 焦云杰 董炫疆 王东宇 杨德博 王华
硅酸盐通报2024,Vol.43Issue(9) :3399-3406.

高熵烧绿石(La1/6 Pr1/6 Nd1/6 Sm1/6 Eu1/6 Gd1/6)2 Zr2O7固化锕系核素的结构和化学稳定性研究

Structure and Chemical Durability of Actinide Nuclides Solidified by High-Entropy Pyrochlore(La1/6Pr1/6Nd1/6Sm1/6Eu1/6Gd1/6)2Zr2O7

杜瞻远 1朱永昌 1崔竹 1焦云杰 1董炫疆 1王东宇 1杨德博 1王华1
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作者信息

  • 1. 中国建筑材料科学研究总院有限公司,北京 100024
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摘要

高熵陶瓷(HECs)具有优异的相稳定性和化学稳定性,是一种潜在的高放废物固化基材.本文设计了一种高熵稀土锆酸盐烧绿石固化基材(La1/6Pr1/6Nd1/6Sm1/6Eu1/6Gd1/6)2Zr2O7,用镧系元素铈(Ce)模拟放射性的锕系核素,采用高温固相法成功制备了一系列固化Ce4+的(La1/6Pr1/6Nd1/6Sm1/6Eu1/6Gd1/6)2(Zr1-XCeX)2O7(0≤X≤0.5)陶瓷固化体,并对固化体的物相组成、微观结构、微观形貌、抗浸出性能进行了测试.结果表明:所有模拟核素皆均匀地固溶进晶体结构中;随着CeO2含量增加,晶体结构由有序烧绿石结构转变为缺陷萤石结构;Ce元素归一化浸出率处于10-7~10-6 g·m-2·d-1,表现出优异的化学稳定性.

Abstract

High-entropy ceramics(HECs)are a potential target for high-level waste curing due to their excellent phase and chemical stability.In this work,a high-entropy rare-earth zirconate pyrochlore(La1/6Pr1/6Nd1/6Sm1/6Eu1/6Gd1/6)2Zr2O7 was designed.And the lanthanide element Ce was used as simulated radioactive actinide nuclides.A series of ceramic solidifications(La1/6Pr1/6 Nd1/6 Sm1/6 Eu1/6 Gd1/6)2(Zr1-XCex)2O7(0≤X≤0.5)were prepared using a high temperature solid phase method to solidify Ce.The solidifying performances were evaluated by analyzing the physical phase composition,microstructure,microscopic morphology,and anti-leaching.The results show that all the nuclides are uniformly solidly dissolved into crystal structure.As the CeO2 content increases,the crystal structure changes from an ordered pyrochlore phase to a defective fluorite phase.The normalized leaching rates of Ce range from 10-7 g·m-2·d-1 to10-6g·m-2·d-1,showing excellent chemical stability.

关键词

高熵陶瓷/高熵烧绿石/高放废物/陶瓷固化/化学稳定性

Key words

high-entropy ceramics/high-entropy pyrochlore/high-level waste/ceramic solidification/chemical durability

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出版年

2024
硅酸盐通报
中国硅酸盐学会 中材人工晶体研究院

硅酸盐通报

CSTPCD北大核心
影响因子:0.698
ISSN:1001-1625
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