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

Journal 2022 · IF 16.744 · 发表于 2022 年 1 月 11 日
作者: Zhongyue Li,Ruomeng Zhu,Pengling Zhang,Mei Yang,Ruiqi Zhao,Yanlong Wang,Xing Dai,Wei Liu
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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 (Q m ) 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 (C 0  = 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 (Q m  = 4604 μg⋅g −1 ) from real seawater. U L 3 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 η 2 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.

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