Efficient Removal and Recovery of Uranium by a Layered Organic-Inorganic Hybrid Thiostannate

被引:350
作者
Feng, Mei-Ling [1 ,2 ]
Sarma, Debajit [2 ]
Qi, Xing-Hui [1 ]
Du, Ke-Zhao [1 ]
Huang, Xiao-Ying [1 ]
Kanatzidis, Mercouri G. [2 ]
机构
[1] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
[2] Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA
基金
美国国家科学基金会;
关键词
ION-EXCHANGE; AQUEOUS-SOLUTIONS; METAL SULFIDES; URANYL IONS; WASTE-WATER; ADSORPTION; EXTRACTION; CHEMISTRY; FRAMEWORK; SORBENTS;
D O I
10.1021/jacs.6b07351
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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.
引用
收藏
页码:12578 / 12585
页数:8
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