文献类型：期刊文献

英文题名：Phosphonate-Decorated Covalent Organic Frameworks for Actinide Extraction: A Breakthrough Under Highly Acidic Conditions

作者：Yu, Jipan[1];Yuan, Liyong[1];Wang, Shuai[1,2];Lan, Jianhui[1];Zheng, Lirong[3];Xu, Chao[4];Chen, Jing[4];Wang, Lin[1];Huang, Zhiwei[1];Tao, Wuqing[1];Liu, Zhirong[2];Chai, Zhifang[1];Gibson, John K.[5];Shi, Weiqun[1]

机构：[1]Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China;[2]East China Univ Sci & Technol, Coll Nucl Sci & Engn, Nanchang 330013, Jiangxi, Peoples R China;[3]Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China;[4]Tsinghua Univ, Collaborat Innovat Ctr Adv Nucl Energy Technol, Inst Nucl & New Energy Technol INET, Beijing 100084, Peoples R China;[5]LBNL, Chem Sci Div, Berkeley, CA 94720 USA

年份：2019

卷号：1

期号：3

起止页码：286

外文期刊名：CCS CHEMISTRY

收录：WOS:【ESCI(收录号:WOS:000787310300006)】；

基金：This work was supported by the National Natural Science Foundation of China (Grant Nos. 21577144, 21777161, 11575212, and 21806167), the Science Challenge Project (TZ2016004), and the Youth Innovation Promotion Association of CAS (2017020). The theoretical results described in this work were obtained on the platform of Supercomputing Center, Computer Network Information Center of Chinese Academy of Sciences. Research of JKG was supported by the Center for Actinide Science and Technology, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award Number DE-SC0016568.

语种：英文

外文关键词：COFs; solid-phase extraction; uranium; plutonium; highly acidic conditions

摘要：Although solid-phase extraction is a useful approach for metal ion separation from aqueous solutions, existing sorbents suffer from low extraction efficiencies and/or instability when in contact with strong acidic media. We report here the first study on rational design and fabrication of phosphonate-decorated covalent organic frameworks, COF-IHEP1 and COF-IHEP2, for efficient and selective extraction of of uranium (VI) [U(VI)] and plutonium(IV) [Pu(IV)] from highly acidic solutions. We found that the negatively charged frameworks with excellent stability under harsh conditions and strong chelating ability from incorporated phosphonate moieties make the COFs superb U(VI) and Pu(IV) sorbents. In 1 M HNO3 solution, COF-IHEP1 achieved recorded U(VI) uptake of 112 mg.g(-1), with extremely high selectivity toward Pu(IV) even in the presence of large excess of competing metal cations. Our mechanistic study con- firms a sandwich-type microstructure of hydrated U(VI) and Pu(IV) cations bound by the oxygen sites of phosphonate groups. These newly fabricated tailored hybrid porous materials could afford new opportunities to achieve highly efficient actinide extraction from acidic nuclear fuel effluents. [GRAPHICS] .