Efficient Removal and Recovery of Uranium by a Layered Organic-Inorganic Hybrid Thiostannate
Efficient Removal and Recovery of Uranium by a Layered Organic-Inorganic Hybrid Thiostannate
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层状有机-无机杂化硫锡酸盐高效去除和回收铀
DOI：
10.1021/jacs.6b07351
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发表时间：
2016-09-28
影响因子：
15
通讯作者：
Kanatzidis, Mercouri G.
中科院分区：
文献类型：
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作者：
Feng, Mei-Ling;Sarma, Debajit;Kanatzidis, Mercouri G.
铀在核燃料循环中既作为能源又作为放射性废物很重要。从核废料溶液中回收铀进行进一步处理和处置至关重要。在此，我们提出了第一硫属化物实例，（Me 2NH 2）（1.33）（Me 3 NH）（0.67）Sn 3S 7中心点1.25H（2）O（FJSM-SnS），其中有机胺阳离子可用于选择性UO 22 +-离子交换。UO_（22+）交换动力学完全符合准二级反应，这是在硫属离子交换剂中首次观察到的。揭示了化学吸附过程及其离子交换机理。FJSM-SnS在强酸性和强碱性环境（pH = 2.1-11）中均具有优异的pH稳定性，最大铀交换容量为338.43 mg/g。在高浓度的Na+、Ca ~（2+）或HCO ~（3-）存在下，它能有效地捕获UO ~（2+）离子（最高分配系数K-d值达4.28 × 10 ~（4）mL/g）。在存在过量Na+的情况下，该材料在去除痕量水平的U方面也非常有效（去除的U的相对量接近100%）。UO 22+中心点S2-相互作用是高选择性的基础。重要的是，交换产物中的铀酰离子可以很容易地用环境友好的方法洗脱，通过用浓缩的KCl溶液处理UO 22+负载的材料。这些优点加上非常高的负载能力，低成本，环境友好的性质，和易于合成，使FJSM-SnS一个新的有前途的修复材料，从核废料溶液中去除放射性U。
Uranium is important in the nuclear fuel cycle both as an energy source and as radioactive waste. It is of vital importance to recover uranium from nuclear waste solutions for further treatment and disposal. Herein we present the first chalcogenide example, (Me2NH2)(1.33)(Me3NH)(0.67)Sn3S7 center dot 1.25H(2)O (FJSM-SnS), in which organic amine cations can be used for selective UO22+-ion-exchange. The UO22+-exchange kinetics perfectly conforms to pseudo-second-order reaction, which is observed for the first time in a chalcogenide ion-exchanger. This reveals the chemical adsorption process and its ion-exchange mechanism. FJSM-SnS has excellent pH stability in both strongly acidic and basic environments (pH = 2.1-11), with a maximum uranium-exchange capacity of 338.43 mg/g. It can efficiently capture UO22+ ions in the presence of high concentrations of Na+, Ca2+, or HCO3- (the highest distribution coefficient K-d value reached 4.28 X 10(4) mL/g). The material is also very effective in removing of trace levels of U in the presence of excess Na+ (the relative amounts of U removed are close to 100%). The UO22+center dot center dot center dot S2- interactions are the basis for the high selectivity. Importantly, the uranyl ion in the exchanged products could be easily eluted with an environmentally friendly method, by treating the UO22+-laden materials with a concentrated KCl solution. These advantages coupled with the very high loading capacity, low cost, environmentally friendly nature, and facile synthesis make FJSM-SnS a new promising remediation material for removal of radioactive U from nuclear waste solutions.