Utilizing Ionic Liquids as Bifunctional Reagents for the Ionothermal Synthesis of Uranyl Compounds
Utilizing Ionic Liquids as Bifunctional Reagents for the Ionothermal Synthesis of Uranyl Compounds
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DOI：
10.1021/acs.cgd.3c00976
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发表时间：
2023-10-10
影响因子：
3.8
通讯作者：
Burns，Peter C.
中科院分区：
文献类型：
--
作者：
Felton，Daniel E.;Kohlgruber，Tsuyoshi A.;Burns，Peter C.
从裂变产物中提取锕系元素，特别是铀酰和其他锕系离子是乏核燃料后处理的一个关键方面。在这项研究中，进行离子热合成来控制通过暴露于一系列离子液体（IL）而产生的铀酰（UO2）2+盐复合物的形成。通过连接 IL 阴离子组分，同时提供极性反应介质以促进形态形成，以多方面的方法利用 IL 的高热稳定性和连接潜力来实现铀酰盐络合。此外，通过 IL 阳离子对铀酰络合物模板的评估表明，小的杂环阳离子分子会产生更密集的阴离子簇。还改变了铀源以确定硝酸盐对离子液体的氧化作用以及硝酸盐和乙酸盐副产物形成的倾向。三氟甲磺酸铀酰被发现是生产纯铀酰络合物的最佳铀源。研究了硝酸盐氧化离子液体的程度，以确定形成什么氧化产物并随后与铀酰离子配位。最后，结果表明，可以从含有琥珀酸根阴离子的离子液体中高产率合成琥珀酸双氧铀骨架。
The extraction of actinides, specifically uranyl and other actinyl ions, from fission products is a critical aspect of spent nuclear fuel reprocessing. In this study, ionothermal syntheses were conducted to control the formation of uranyl (UO2)2+salt complexes generated by exposure to a selection of ionic liquids (ILs). The high-thermal stability and ligation potential of ILs were exploited in a multifaceted approach toward uranyl salt complexation by enabling ligation of the IL anionic component while simultaneously providing polar reaction media to promote speciation. Furthermore, an evaluation of uranyl complex templating by the IL cation revealed that small, heterocyclic cationic molecules resulted in more densely packed anionic clusters. The uranium source was also varied to determine the oxidizing effect of nitrate on the ILs and the propensity for nitrate and acetate byproduct formation. Uranyl triflate was found to be the optimal uranium source for the production of pure uranyl complexes. The degree to which nitrate oxidizes the ILs was investigated to determine what oxidation products form and subsequently coordinate to the uranyl ion. Finally, it was shown that a uranyl succinate framework can be synthesized in high yield from an IL that contains succinate as the anion.