Xie Xiang, Qin Zhen, He Yao, Xiong Penghui, Huang Zeng, Mao Yiwu, Wei Hongyuan, Zhuo Liangang
Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang, 621900, China.
Institute of Materials, China Academy of Engineering Physics, Mianyang, 621900, China.
Sci Rep. 2017 Nov 16;7(1):15735. doi: 10.1038/s41598-017-15899-0.
The influence of the linking group between the phosphoryl and bridging moieties in phosphoryl-containing task-specific ionic liquids (TSILs) on the extraction of uranyl ions was experimentally and theoretically investigated. A novel phosphoramidate-based TSIL with an amine group as the linking moiety resulted in a higher uranyl ion extraction efficiency compared with that of other phosphoryl-based TSILs. A distribution ratio of 4999 ± 51 can be achieved for uranyl ions. The uranyl ions (76.7 ± 1.5%) were stripped from the loaded ionic liquid phase in a single stage using 0.05 M diethylenetriamine pentaacetic acid in a 1.0 M guanidine carbonate solution. The extraction stoichiometry of the uranyl ions was determined by a slope analysis of the extraction data. Furthermore, the fundamental nature of the interaction between the phosphoramidate-based TSIL and uranyl ions was theoretically studied for the first time. The theoretical calculations demonstrated that the synergistic effect of the complexation interaction and H-bond formation between the phosphoramidate-functional ionic liquid and uranyl nitrate led to the higher extraction efficiency. These results provide a basis for rational design, synthesis and potential applications of novel TSILs for uranyl extraction.
实验和理论研究了含磷特定任务离子液体(TSILs)中磷酰基和桥连部分之间的连接基团对铀酰离子萃取的影响。一种以胺基为连接基团的新型氨基磷酸酯基TSIL与其他基于磷酰基的TSIL相比,具有更高的铀酰离子萃取效率。铀酰离子的分配比可达4999±51。使用1.0 M碳酸胍溶液中的0.05 M二乙烯三胺五乙酸在单级中从负载离子液相中反萃出76.7±1.5%的铀酰离子。通过对萃取数据的斜率分析确定了铀酰离子的萃取化学计量。此外,首次从理论上研究了氨基磷酸酯基TSIL与铀酰离子之间相互作用的基本性质。理论计算表明,氨基磷酸酯功能化离子液体与硝酸铀酰之间的络合相互作用和氢键形成的协同效应导致了更高的萃取效率。这些结果为新型TSILs用于铀酰萃取的合理设计、合成及潜在应用提供了依据。