Ionic liquids with polychloride anions as effective oxidants for the dissolution of UO2.
Ionic liquids with polychloride anions as effective oxidants for the dissolution of UO2.
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含有多氯阴离子的离子液体作为溶解UO2的有效氧化剂。
DOI：
10.1039/c9dt03574e
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发表时间：
2019-11
影响因子：
4
通讯作者：
Taiwei Chu
中科院分区：
文献类型：
--
作者：
Aining Yao;Feng Qu;Yu Liu;Guangyin Qu;Hao Lin;Shaowen Hu;Xiangyun Wang;Taiwei Chu
本文以氯化咪唑盐为前驱体，通过通入氯气制备了聚氯离子液体（[Cl 3]-或[Cl 5]-）。在六种咪唑鎓氯化物[Rmim]Cl（Rmim = Almim，1-乙基-3-甲基咪唑鎓; Bmim，1-丁基-3-甲基咪唑鎓; Pmim，1-丙基-3-甲基咪唑鎓; Pnmim，1-戊基-3-甲基咪唑鎓; Hmim，1-己基-3-甲基咪唑鎓;和Omim，1-辛基-3-甲基咪唑鎓）中，在[Bmim]Cl IL中发现Cl 2的最高储存能力。当使用[Bmim][Tf 2N]（1-丁基-3-甲基咪唑双三氟甲酰胺）和[Bmim]Cl的混合离子液体时，离子液体阳离子在氯化过程中保持良好的稳定性，并且根据1H NMR光谱，咪唑阳离子[Bmim]+在引入氯气后几乎保持相同的结构。实验结果表明，所合成的多氯离子液体不仅能成功地溶解UO 2，而且能降低Cl 2的消耗，提高氯效率。光谱研究表明，[UO 2Cl 4]2-是离子液体反应的主要产物。溶解的铀酰物质可以通过结晶以[Bmim]2[UO 2Cl 4]的形式容易地从离子液体中回收。此外，即使与溶解的铀和镧系元素的总量相比，57.1重量%的镧系元素溶解在IL混合物中，也只能从体系中分离出含铀晶体。
Herein, polychloride ([Cl3]- or/and [Cl5]-) ionic liquids (ILs) were prepared from their imidazolium chloride precursors by the addition of chlorine gas. The highest storage ability of Cl2 was found in the [Bmim]Cl IL among the six imidazolium chlorides [Rmim]Cl (Rmim = Emim, 1-ethyl-3-methylimidazolium; Bmim, 1-butyl-3-methylimidazolium; Pmim, 1-propyl-3-methylimidazolium; Pnmim, 1-pentyl-3-methylimidazolium; Hmim, 1-hexyl-3-methylimidazolium; and Omim, 1-octyl-3-methylimidazolium). When a mixed IL of [Bmim][Tf2N] (1-butyl-3-methylimidazolium bistriflimide) and [Bmim]Cl was used, the IL cation could maintain good stability during the chlorination process, and the imidazolium cation [Bmim]+ could retain almost the same structure after the chlorine gas was introduced into the mixed IL according to 1H NMR spectroscopy. It has been found that the synthesized polychloride ILs not only can successfully dissolve UO2, but can also decrease the consumption of Cl2 and increase the chlorine efficiency. Spectroscopy studies indicate that [UO2Cl4]2- is the principal product in the IL reaction solution. The dissolved uranyl species can be easily recovered from the ILs by crystallization in the form of [Bmim]2[UO2Cl4]. Moreover, even if 57.1 wt% of the lanthanide element, when compared with the total amount of dissolved uranium and lanthanide elements, was dissolved in the IL mixture, only uranium-containing crystals could be isolated from the system.
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影响因子：
1.2
作者：
O. Tomioka;Y. Meguro;Y. Enokida;I. Yamamoto;Z. Yoshida
通讯作者：
O. Tomioka;Y. Meguro;Y. Enokida;I. Yamamoto;Z. Yoshida
影响因子：
4
作者：
Maggel Deetlefs;C. Hussey;T. Mohammed;K. R. Seddon;J. van den Berg;J. A. Zora
通讯作者：
Maggel Deetlefs;C. Hussey;T. Mohammed;K. R. Seddon;J. van den Berg;J. A. Zora
影响因子：
4.6
作者：
S. Pasilis;J. Pemberton
通讯作者：
S. Pasilis;J. Pemberton
影响因子：
4.6
作者：
Clare E Rowland;Mercouri G Kanatzidis;L. Soderholm
通讯作者：
Clare E Rowland;Mercouri G Kanatzidis;L. Soderholm
影响因子：
4.6
作者：
Fan, Fang-Li;Qin, Zhi;Feng, Xiao-Gui
通讯作者：
Feng, Xiao-Gui