Zhou Lin, Li Fei, Liu Ji-Xuan, Sun Shi-Kuan, Liang Yongcheng, Zhang Guo-Jun
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, College of Science, Institute of Functional Materials, Donghua University, Shanghai 201620, China.
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, College of Science, Institute of Functional Materials, Donghua University, Shanghai 201620, China.
J Hazard Mater. 2021 Aug 5;415:125596. doi: 10.1016/j.jhazmat.2021.125596. Epub 2021 Mar 8.
The sustainable development of civil nuclear energy requires the fabrication of the durable nuclear wasteforms, in particular for high-level radioactive waste, which involves the design of the composition and microstructure. Herein, we demonstrated that high-entropy ceramics (EuGd)(TiZrHfNbCe)O are the potential candidate as immobilizing hosts for high-level radioactive waste. The static aqueous leaching test indicates that the normalized leaching rates for the simulated radionuclides Ce (LR) and Gd (LR) in as-prepared high-entropy ceramics are approximately 1010 g·m·d after 42 days testing, much lower than those reported values in doped-GdZrO (1010 g·m·d). The excellent chemical durability is mainly due to the synergistic effects of the compositional complexity and severe lattice distortion. Compared to their ternary oxides, the low oxygen vacancy concentration slows down the migration and diffusion of cations. Moreover, the lattice distortion increases the lattice potential energy, also inhibiting the migration of cations. This study provides a strategy for the development and application of high-entropy ceramics as the wasteforms.
民用核能的可持续发展需要制造耐用的核废料固化体,特别是对于高放废物,这涉及到成分和微观结构的设计。在此,我们证明了高熵陶瓷(EuGd)(TiZrHfNbCe)O是作为高放废物固定主体的潜在候选材料。静态水浸试验表明,在42天的测试后,所制备的高熵陶瓷中模拟放射性核素Ce(LR)和Gd(LR)的归一化浸出率约为1010 g·m·d,远低于掺杂GdZrO中报道的值(1010 g·m·d)。优异的化学耐久性主要归因于成分复杂性和严重晶格畸变的协同效应。与它们的三元氧化物相比,低氧空位浓度减缓了阳离子的迁移和扩散。此外,晶格畸变增加了晶格势能,也抑制了阳离子的迁移。本研究为高熵陶瓷作为废料固化体的开发和应用提供了一种策略。