新型功能化共价-有机骨架材料的设计、合成及其对176Yb/177Lu的选择性分离行为与机理研究

177Lu是最具临床应用价值和市场前景的肿瘤诊疗核素之一。176Yb-177Lu的高效选择性分离是制备无载体177Lu的关键，但国外现有分离材料与方法仍然存在效率偏低、机理模糊、工艺复杂或引入二次污染物等不足，而国内尚未见相关研究报道。为此，本项目拟以理论计算与实验结合的方式开展新型共价-有机框架(COFs)材料的设计、合成及其对Yb/Lu的分离行为与机理研究。通过COFs单体设计与Yb/Lu螯合能力、材料结构设计与理化性质计算、材料对Lu吸附行为与机理及177Lu柱分离流程构建等内容的开展，确定基于理论计算的COFs设计与制备新方法，获得稳定性高、分离性能优良的新型COFs材料，揭示其对Lu选择性吸附的机理，并在此基础上建立基于COFs材料的无载体177Lu分离工艺流程。项目的实施不仅可为176Yb-177Lu的分离提供新的思路，对我国无载体177Lu的自主化生产也将起到良好的推动作用。

Lutetium-177 has been regarded as one of the most valuable radionuclides which possess highly-promising applications in the tumor-targeted diagnosis and treatment. Selective separation of lutetium-177 from enriched ytterbium-176 with high efficiency is the key to the preparation of non-carrier added 177Lu. However, the previously reported separation methods and the related materials still have some disadvantages, such as low efficiency, ambiguous mechanism, complicated process or contamination of extra pollutants. Motivated by this, the present project is proposing to achieve rational design and synthesis of new covalent-organic frameworks (COFs) by combining theoretical calculation and plenty of experimental studies, which will also determine the adsorption behavior and separation mechanism of 176Yb-177Lu by obtained COFs. The main contents include: 1) theoretical design of the COFs monomers and calculation of their chelating ability with Lu3+, along with the determination of materials’ micro structures and physicochemical properties; 2) preparation, characterization and chemical, mechanical and irradiation stability of the obtained COFs; 3) adsorption behavior and separation mechanism of Lu3+ by COFs; 4) establishment of the chromatography separation process of 177Lu from the solution practical irradiated target. After this project finished, a new preparation method of COFs based on theoretical calculations and practical experiments will be determined, and some novel functional materials with excellent separation performance for Lu will be obtained. Additionally, the adsorption behavior and separation mechanism of Lu will be addressed. More importantly, the chromatography separation process of non-carrier added 177Lu will be established. We believe this project will not only provide new ideas for the separation of 177Lu from enriched ytterbium-176 with high efficiency and excellent selectivity, but also dramatically promote the independent production of non-carrier added 177Lu in China.