Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 39, Pages 16538-16545Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c08048
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Funding
- National Science Fund for Distinguished Young Scholars [21925603]
- National Natural Science Foundation of China [11875057, 21671191, 21906020]
- Youth Innovation Promotion Association of CAS [2020014]
- U.S. Department of Energy, Office of Basic Energy Sciences, Heavy Element Chemistry Program at LBNL [DE-AC02-05CH11231]
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The separation of actinides has a vital place in nuclear fuel reprocessing, recovery of radionuclides, and remediation of environmental contamination. Here we propose a new paradigm of nanocluster-based actinide separation, namely, nanoextraction, that can achieve efficient sequestration of uranium in an unprecedented form of giant coordination nanocages using a cone-shaped macrocyclic pyrogallol[4]arene as the extractant. The U-24-based hexameric pyrogallol[4]arene nanocages with distinctive [U-2(PG)(2)] binuclear units (PG = pyrogallol) that rapidly assembled in situ in monophasic solvent were identified by single-crystal X-ray diffraction, MALDI-TOF mass spectrometry, NMR spectroscopy, and small-angle X-ray and neutron scattering. Comprehensive biphasic extraction studies showed that this novel separation strategy has enticing advantages such as fast kinetics, high efficiency, and good selectivity over lanthanides, thereby demonstrating its potential for efficient separation of actinide ions.
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