新型邻菲罗啉修饰杯芳烃席夫碱萃取剂分离锕系离子的理论和实验研究

With the development of nuclear energy, safe disposal of radioactive waste is one of the key factors for the sustainable development of nuclear energy. Since calixarenes possessing the advantages of adjustable cavity, variable conformation, and easy modification, they have important application in the separation of radionuclides. This project aims to design and synthesize highly efficient calixarene extractants with phenanthroline ligand and Schiff base functional ligands for extraction of actinides by using multiscale theoretical methods and experimental techniques. To explore highly efficient ligands for separating actinides, the functional groups of calixarenes will be optimized firstly at the atomic and molecular level. And then, novel calixarene extractants will be synthesized experimentally, and the interaction mechanism of actinides and these calixarene ligands will be studied. Combining computational chemistry and experimental techniques, we will mainly focus on the extraction and separation behavior of these extractants for actinides, and the relationship of geometry and extraction properties of the calixarene extractants. It is expected that this project will provide valuable clues for establishing the initial basis for calixarenes application in spent nuclear fuel reprocessing.

随着核能的发展，放射性废物的妥善处理和处置成为制约核能可持续发展的关键因素之一。由于杯芳烃具有空腔可调、构象可变、易于修饰等优点，在放射性核素的分离方面具有重要的应用前景。本项目拟以杯芳烃为基体材料，将高效锕系组分离邻菲罗啉类配体和席夫碱功能配体引入其中，并结合多尺度模拟方法设计合成高效选择性分离锕系离子的新型邻菲罗啉修饰杯芳烃席夫碱萃取剂。首先对杯芳烃的功能基团进行优化设计，从原子和分子水平筛选杯芳烃萃取剂的结构。在此基础上，通过实验合成高效杯芳烃萃取剂，并研究其与锕系离子的相互作用机理，同时结合理论模拟研究新型杯芳烃萃取剂对锕系离子的萃取和分离行为，揭示萃取剂结构与萃取性能及选择性之间的关系，为此类萃取剂在乏燃料后处理方面的应用提供依据。

随着核能的发展，放射性废物的妥善处理和处置成为制约核能可持续发展的关键因素之一。由于杯芳烃具有空腔可调、构象可变、易于修饰等优点，在放射性核素的分离方面具有重要的应用前景。在过去的四年中，我们对邻菲罗啉和酰胺类功能基团进行优化设计，并从实验与理论研究两方面系统研究它们对代表性镧锕离子的萃取行为与作用机制。在此基础上，设计了功能化的杯芳烃萃取剂，研究了萃取产物的结构和成键性质，以及萃取剂对锕系离子的分离行为和机理。这些研究工作丰富了杯芳烃萃取剂在锕系元素分离方面的应用，并为核燃料循环先进技术开发提供了参考。