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Dalton Trans. 2016 Dec 6;45(48):19299-19310.

Highly efficient extraction of actinides with pillar[5]arene-derived diglycolamides in ionic liquids via a unique mechanism involving competitive host-guest interactions.

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College of Chemistry, Institute of Nuclear Science and Technology, Key Laboratory for Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu 610064, China.
Radiochemistry Division, Bhabha Atomic Research Centre, Trombay, Mumbai-400085, India.
Institute of Bioengineering and Nanotechnology, 31 Biopolis Way, The Nanos, Singapore 138669, Singapore.


Actinide partitioning is considered as one of the most challenging issues in nuclear waste remediation. Herein, we unravel a novel extraction mode pertinent to the competitive host-guest interactions for highly efficient actinide extraction. The host-guest recognition event involves binding of a room temperature ionic liquid (RTIL), 1-n-octyl-3 methylimidazolium bis(trifluoromethane)sulfonamide (C8mimNTf2), as both the guest and the solvent by the hosts pillar[5]arene-based diglycolamides (P5DGAs) and the subsequent displacement of the guest by a metal ion. This two-step process suggests a unique competitive ion-mediated displacement mechanism for the metal ion partitioning in the extraction process. The supramolecular extraction system is evaluated for its extraction abilities towards actinide ions such as UO22+, PuO22+, Pu4+, Am3+, and fission product elements such as Eu3+, Sr2+, Cs+. The results demonstrate the exceedingly high distribution ratios and favorable separation of Am3+ and Pu4+ in nitric acid media. All the three P5DGAs form 1 : 1 complexes with Am3+. Time resolved laser fluorescence spectroscopic (TRLFS) studies reveal a strong complexation involving no inner-sphere water molecules in the Eu3+-P5DGA complexes when C8mimNTf2 is used as the diluent. With high efficiency in the extraction of actinides and a quantitative back extraction outcome, the RTIL-based solvent systems containing pillar[5]arene-DGA ligands developed in this work hold potential as promising candidates for nuclear waste remediation in a more sustainable fashion.


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