Liu Xiaojuan, Gao Feng, Jin Tiantian, Ma Ke, Shi Haijiang, Wang Ming, Gao Yanan, Xue Wenjuan, Zhao Jing, Xiao Songtao, Ouyang Yinggen, Ye Guoan
Department of Radiochemistry, China Institute of Atomic Energy, 102413, Beijing, China.
Key Laboratory of Ministry of Education for Advanced Materials in Tropical Island Resources, Hainan University, 570228, Haikou, China.
Nat Commun. 2023 Aug 22;14(1):5097. doi: 10.1038/s41467-023-40704-0.
The selective separation of thorium from rare earth elements and uranium is a critical part of the development and application of thorium nuclear energy in the future. To better understand the role of different N sites on the selective capture of Th(IV), we design an ionic COF named Py-TFImI-25 COF and its deionization analog named Py-TFIm-25 COF, both of which exhibit record-high separation factors ranging from 10 to 10. Py-TFIm-25 COF exhibits a significantly higher Th(IV) uptake capacity and adsorption rate than Py-TFImI-25 COF, which also outperforms the majority of previously reported adsorbents. The selective capture of Py-TFImI-25 COF and Py-TFIm-25 COF on thorium is via Th-N coordination interaction. The prioritization of Th(IV) binding at different N sites and the mechanism of selective coordination are then investigated. This work provides an in-depth insight into the relationship between structure and performance, which can provide positive feedback on the design of novel adsorbents for this field.
从稀土元素和铀中选择性分离钍是未来钍核能开发与应用的关键环节。为了更好地理解不同氮位点在选择性捕获Th(IV)中的作用，我们设计了一种离子型共价有机框架（COF），名为Py-TFImI-25 COF及其去离子化类似物Py-TFIm-25 COF，二者均展现出高达10至10的创纪录分离因子。Py-TFIm-25 COF表现出比Py-TFImI-25 COF显著更高的Th(IV)吸附容量和吸附速率，这也优于大多数先前报道的吸附剂。Py-TFImI-25 COF和Py-TFIm-25 COF对钍的选择性捕获是通过Th-N配位相互作用实现的。随后研究了不同氮位点上Th(IV)结合的优先级以及选择性配位机制。这项工作深入洞察了结构与性能之间的关系，可为该领域新型吸附剂的设计提供积极反馈。
