Functionalized polyarylether-based COFs for rapid and selective extraction of uranium from aqueous solution

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作者
Li, Zhongyue [1 ]
Zhu, Ruomeng [1 ]
Zhang, Pengling [1 ]
Yang, Mei [1 ]
Zhao, Ruiqi [3 ]
Wang, Yanlong [2 ]
Dai, Xing [2 ]
Liu, Wei [1 ]
机构
[1] School of Environmental and Material Engineering, Yantai University, Yantai,Shandong,264005, China
[2] State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, 199 Ren'ai Roa
[3] Henan Key Laboratory of Materials on Deep-Earth Engineering, School of Materials Science and Engineering, Henan Polytechnic University, Jiaozuo,Henan,454000, China
基金
中国国家自然科学基金;
关键词
Metal ions - Uranium compounds - Extraction - Adsorption - Hydrogen bonds - Density functional theory - Seawater - X ray absorption;
D O I
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学科分类号
摘要
Selective uranium extraction from aqueous solution is critical for both radioactive contamination remediation and uranium recovery from seawater. Herein, amidoxime (−AO) and carboxyl (–COOH) groups are equipped on a polyarylether-based covalent organic framework (COF) for fabrication of post-modified adsorbents, JUC-505-AO and JUC-505-COOH. The maximum adsorption capacities (Qm) of JUC-505-AO and JUC-505-COOH are 395 mg⋅g−1 and 464 mg⋅g−1, respectively. JUC-505-COOH shows preponderant uranium extraction efficiencies of 36–95% at low pH 2–4, and its removal performances are almost unaffected at high temperature ranging from 25 to 80 °C. Whereas, JUC-505-AO exhibits an impressive adsorption kinetics with the adsorption process equilibrates within 20 min (C0 = 20 mg⋅L-1), and marked sorption selectivity toward uranium against coexisting metal ions. JUC-505-AO also capable of extracting uranium with fast kinetics and capacity (Qm = 4604 μg⋅g−1) from real seawater. U L3 edge X-ray absorption spectra analysis reveals that uranyl ions in JUC-505-AO are anchored by coordinating with O and N from the oxime groups by η2 mode with the coordination numbers of 5 or 6. Meanwhile, HOH⋅⋅⋅O hydrogen bonds between the coordinated water of the hydrated uranyl ions and the oxygen atoms on the skeleton of JUC-505-AO were observed by density functional theory simulations. © 2022
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