Task-Specific Tailored Cationic Polymeric Network with High Base-Resistance for Unprecedented 99TcO4- Cleanup from Alkaline Nuclear Waste

被引:145
作者
Li, Jie [1 ,2 ]
Li, Baoyu [1 ,2 ]
Shen, Nannan [1 ,2 ]
Chen, Lixi [1 ,2 ]
Guo, Qi [1 ,2 ]
Chen, Long [1 ,2 ]
He, Linwei [1 ,2 ]
Dai, Xing [1 ,2 ]
Chai, Zhifang [1 ,2 ]
Wang, Shuao [1 ,2 ]
机构
[1] Soochow Univ, State Key Lab Radiat Med & Protect, Sch Radiol & Interdisciplinary Sci RAD X, Suzhou 215123, Peoples R China
[2] Soochow Univ, Collaborat Innovat Ctr Radiat Med Jiangsu Higher, Suzhou 215123, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
COVALENT ORGANIC FRAMEWORK; STABILITY; EXTRACTION; HYDROXIDE; TC-99; RIVER; IMMOBILIZATION; PERTECHNETATE; RHENIUM(VII); ADSORPTION;
D O I
10.1021/acscentsci.1c00847
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Direct removal of (TcO4-)-Tc-99 from alkaline nuclear waste is desirable because of the nuclear waste management and environmental protection relevant to nuclear energy but is yet to be achieved given that combined features of decent base-resistance and high uptake selectivity toward anions with low charge density have not been integrated into a single anion-exchange material. Herein, we proposed a strategy overcoming these challenges by rationally modifying the imidazolium unit of a cationic polymeric network (SCU-CPN-4) with bulky alkyl groups avoiding its ring-opening reaction induced by OH- because of the steric hindrance effect. This significantly improves not only the base-resistance but also the affinity toward TcO4- as a result of enhanced hydrophobicity, compared to other existing anion-exchange materials. More importantly, SCU-CPN-4 exhibits record high uptake selectivity, fast sorption kinetics, sufficient robustness, and promising reusability for removing (TcO4-)-Tc-99 from the simulated high-level waste stream at the U.S. Savannah River Site, a typical alkaline nuclear waste, in both batch experiment and dynamic column separation test for the first time.
引用
收藏
页码:1441 / 1450
页数:10
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