Universität zu Köln

Yaprak, Damla, Spielberg, Eike T., Baecker, Tobias, Richter, Mark, Mallick, Bert, Klein, Axel ORCID: 0000-0003-0093-9619 and Mudring, Anja-Verena (2014). A Roadmap to Uranium Ionic Liquids: Anti-Crystal Engineering. Chem.-Eur. J., 20 (21). S. 6482 - 6494. WEINHEIM: WILEY-V C H VERLAG GMBH. ISSN 1521-3765

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Abstract

In the search for uranium-based ionic liquids, tris(N,N-dialkyldithiocarbamato)uranylates have been synthesized as salts of the 1-butyl-3-methylimidazolium (C(4)mim) cation. As dithiocarbamate ligands binding to the UO22+ unit, tetra-, penta-, hexa-, and heptamethylenedithiocarbamates, N,N-diethyldithiocarbamate, N-methyl-N-propyldithiocarbamate, N-ethyl-N-propyldithiocarbamate, and N-methyl-N-butyldithiocarbamate have been explored. X-ray single-crystal diffraction allowed unambiguous structural characterization of all compounds except N-methyl-N-butyldithiocarbamate, which is obtained as a glassy material only. In addition, powder X-ray diffraction as well as vibrational and UV/Vis spectroscopy, supported by computational methods, were used to characterize the products. Differential scanning calorimetry was employed to investigate the phase-transition behavior depending on the N,N-dialkyldithiocarbamato ligand with the aim to establish structure-property relationships regarding the ionic liquid formation capability. Compounds with the least symmetric N,N-dialkyldithiocarbamato ligand and hence the least symmetric anions, tris(N-methyl-N-propyldithiocarbamato)uranylate, tris(N-ethyl-N-propyldithiocarbamato)uranylate, and tris(N-methyl-N-butyldithiocarbamato)uranylate, lead to the formation of (room-temperature) ionic liquids, which confirms that low-symmetry ions are indeed suitable to suppress crystallization. These materials combine low melting points, stable complex formation, and hydrophobicity and are therefore excellent candidates for nuclear fuel purification and recovery.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Yaprak, Damla UNSPECIFIED UNSPECIFIED UNSPECIFIED Spielberg, Eike T. UNSPECIFIED UNSPECIFIED UNSPECIFIED Baecker, Tobias UNSPECIFIED UNSPECIFIED UNSPECIFIED Richter, Mark UNSPECIFIED UNSPECIFIED UNSPECIFIED Mallick, Bert UNSPECIFIED UNSPECIFIED UNSPECIFIED Klein, Axel UNSPECIFIED orcid.org/0000-0003-0093-9619 UNSPECIFIED Mudring, Anja-Verena UNSPECIFIED UNSPECIFIED UNSPECIFIED
URN:	urn:nbn:de:hbz:38-438227
DOI:	10.1002/chem.201303333
Journal or Publication Title:	Chem.-Eur. J.
Volume:	20
Number:	21
Page Range:	S. 6482 - 6494
Date:	2014
Publisher:	WILEY-V C H VERLAG GMBH
Place of Publication:	WEINHEIM
ISSN:	1521-3765
Language:	English
Faculty:	Faculty of Mathematics and Natural Sciences
Divisions:	Faculty of Mathematics and Natural Sciences > Department of Chemistry > Institute of Inorganic Chemistry
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language SOLUBILIZING METAL-OXIDES; URANYL COMPLEXES; 1-BUTYL-3-METHYLIMIDAZOLIUM CHLORIDE; BASIS-SETS; SPECTRA; DITHIOCARBAMATE; EXTRACTION; BEHAVIOR; RN Multiple languages Chemistry, Multidisciplinary Multiple languages
Refereed:	Yes
URI:	http://kups.ub.uni-koeln.de/id/eprint/43822