Yang Xiaofan, Xu Lei, Fang Dong, Zhang Anyun, Xiao Chengliang
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310058, China.
Institute of Nuclear-Agricultural Science, Key Laboratory of Nuclear Agricultural Sciences of Ministry of Agriculture and Zhejiang Province, Zhejiang University, Hangzhou 310058, China.
Chem Commun (Camb). 2024 Oct 8;60(81):11415-11433. doi: 10.1039/d4cc03810j.
Spent nuclear fuel (SNF) released from reactors possesses significant radioactivity, heat release properties, and high-value radioactive nuclides. Therefore, using chemical methods for reprocessing can enhance economic efficiency and reduce the potential environmental risks of nuclear energy. Due to the presence of relatively diffuse f-electrons, the chemical properties of trivalent lanthanides (Ln(III)) and actinides (An(III)) in SNF solutions are quite similar. Separation methods have several limitations, including poor separation efficiency and the need for multiple stripping agents. The use of novel multi-dental phenanthroline-derived extractants with nitrogen donor atoms to effectively separate An(III) over Ln(III) has been widely accepted. This review first introduces the development history of phenanthroline-derived extractants for extraction and complexation with An(III) over Ln(III). Then, based on structural differences, these extractants are classified into four categories: nitrogen-coordinated, ,-hybrid coordinated, highly preorganized structure, and unsymmetric structure. Each category's design principles, extraction, and separation performance as well as their advantages and disadvantages are discussed. Finally, we have summarized and compared the unique characteristics of the existing extractants and provided an outlook. This work may offer a reliable reference for the precise identification and selective separation between An(III) and Ln(III), and point the way for future development and exploration.
反应堆中释放出的乏核燃料具有显著的放射性、放热特性和高价值放射性核素。因此,采用化学方法进行后处理可以提高经济效益并降低核能潜在的环境风险。由于存在相对弥散的f电子,乏核燃料溶液中三价镧系元素(Ln(III))和锕系元素(An(III))的化学性质非常相似。分离方法存在若干局限性,包括分离效率低下以及需要多种反萃剂。使用具有氮供体原子的新型多齿菲咯啉衍生萃取剂来有效分离An(III)和Ln(III)已被广泛认可。本综述首先介绍了菲咯啉衍生萃取剂用于萃取以及与An(III)和Ln(III)络合的发展历程。然后,基于结构差异,将这些萃取剂分为四类:氮配位型、π-杂化配位型、高度预组织化结构型和不对称结构型。讨论了每一类的设计原理、萃取和分离性能以及它们的优缺点。最后,我们总结并比较了现有萃取剂的独特特性并给出了展望。这项工作可为An(III)和Ln(III)之间的精确识别和选择性分离提供可靠参考,并为未来的发展和探索指明方向。