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Title: Synthesis of Anhydrous Acetates for the Components of Nuclear Fuel Recycling in Dialkylimidazolium Acetate Ionic Liquids [plus supplemental information]

Abstract

A series of anhydrous acetate salts with uranium {[C2C1im][UO2(OAc)3] (1), [C2C2im][UO2(OAc)3] (2), and [C4C1im][UO2(OAc)3] (3)}, lanthanides {[C2C2im]2[La(OAc)5] (4) and [C2C1im]2[Nd(OAc)5] (5)}, and strontium {[C2C1im]n[Sr- (OAc)3]n (6)} (where C2C1im = 1-ethyl-3-methylimidazolium, C2C2im = 1,3-diethylimidazolium, C4C1im = 1-butyl-3-methylimi-dazolium, and OAc = acetate) have been prepared and structurally characterized. Both lanthanides and strontium are common components of the nuclear fuel waste, and their separation from uranium is an important but still challenging task. A new synthetic method with dialkylimidazolium acetate ionic liquids (ILs) as the solvent has been developed for the direct synthesis of homoleptic acetates from the corresponding hydrates and, unexpectedly, hardly soluble f-element oxides. Although the group of characterized compounds shows perfect structural variability, all actinide and lanthanide metal ions form monomeric complex anions where the metal cation coordinates to five ligands including two oxygen atoms in the case of uranium, as is commonly observed for uranyl compounds. Crystallographic analyses revealed that the complex [UO2(OAc)3]- anions possess rather standard D3h symmetry featuring a hexagonal-bipyramidal coordination environment, while the lanthanide anions [Ln(OAc)5]2- are fully asymmetric and the Ln3+ cations are 10-coordinated in the form of a distorted bicapped tetragonal antiprism. This is the first report of lanthanide ions coordinated in this fashion.more » For Sr2+, 9-fold coordination through oxygen atoms in the form of a strongly distorted tricapped trigonal prism is observed. Furthermore, the crystallization of anhydrous, homoleptic, anionic acetate complexes from such a large variety of different metal salts appears to be due to the properties of dialkylimidazolium acetate ILs themselves, including enhanced basicity from the high concentration of free anions and their greater affinity for hydrogen-bonding solutes relative to metal cations.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [5]
  1. Stockholm Univ. (Sweden)
  2. Univ. of Alabama, Tuscaloosa, AL (United States)
  3. McGill Univ., Montreal, QC (Canada)
  4. Qingdao Agricultural Univ. (China)
  5. Stockholm Univ. (Sweden); Univ. of Alabama, Tuscaloosa, AL (United States); McGill Univ., Montreal, QC (Canada)
Publication Date:
Research Org.:
Univ. of Alabama, Tuscaloosa, AL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Swedish Research Council (SRC)
OSTI Identifier:
1592765
Grant/Contract Number:  
SC0019220
Resource Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 59; Journal Issue: 1; Journal ID: ISSN 0020-1669
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Smetana, Volodymyr, Kelley, Steven P., Titi, Hatem M., Hou, Xiaomin, Tang, Si-Fu, Mudring, Anja-Verena, and Rogers, Robin D. Synthesis of Anhydrous Acetates for the Components of Nuclear Fuel Recycling in Dialkylimidazolium Acetate Ionic Liquids [plus supplemental information]. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.inorgchem.9b03077.
Smetana, Volodymyr, Kelley, Steven P., Titi, Hatem M., Hou, Xiaomin, Tang, Si-Fu, Mudring, Anja-Verena, & Rogers, Robin D. Synthesis of Anhydrous Acetates for the Components of Nuclear Fuel Recycling in Dialkylimidazolium Acetate Ionic Liquids [plus supplemental information]. United States. https://doi.org/10.1021/acs.inorgchem.9b03077
Smetana, Volodymyr, Kelley, Steven P., Titi, Hatem M., Hou, Xiaomin, Tang, Si-Fu, Mudring, Anja-Verena, and Rogers, Robin D. Mon . "Synthesis of Anhydrous Acetates for the Components of Nuclear Fuel Recycling in Dialkylimidazolium Acetate Ionic Liquids [plus supplemental information]". United States. https://doi.org/10.1021/acs.inorgchem.9b03077. https://www.osti.gov/servlets/purl/1592765.
@article{osti_1592765,
title = {Synthesis of Anhydrous Acetates for the Components of Nuclear Fuel Recycling in Dialkylimidazolium Acetate Ionic Liquids [plus supplemental information]},
author = {Smetana, Volodymyr and Kelley, Steven P. and Titi, Hatem M. and Hou, Xiaomin and Tang, Si-Fu and Mudring, Anja-Verena and Rogers, Robin D.},
abstractNote = {A series of anhydrous acetate salts with uranium {[C2C1im][UO2(OAc)3] (1), [C2C2im][UO2(OAc)3] (2), and [C4C1im][UO2(OAc)3] (3)}, lanthanides {[C2C2im]2[La(OAc)5] (4) and [C2C1im]2[Nd(OAc)5] (5)}, and strontium {[C2C1im]n[Sr- (OAc)3]n (6)} (where C2C1im = 1-ethyl-3-methylimidazolium, C2C2im = 1,3-diethylimidazolium, C4C1im = 1-butyl-3-methylimi-dazolium, and OAc = acetate) have been prepared and structurally characterized. Both lanthanides and strontium are common components of the nuclear fuel waste, and their separation from uranium is an important but still challenging task. A new synthetic method with dialkylimidazolium acetate ionic liquids (ILs) as the solvent has been developed for the direct synthesis of homoleptic acetates from the corresponding hydrates and, unexpectedly, hardly soluble f-element oxides. Although the group of characterized compounds shows perfect structural variability, all actinide and lanthanide metal ions form monomeric complex anions where the metal cation coordinates to five ligands including two oxygen atoms in the case of uranium, as is commonly observed for uranyl compounds. Crystallographic analyses revealed that the complex [UO2(OAc)3]- anions possess rather standard D3h symmetry featuring a hexagonal-bipyramidal coordination environment, while the lanthanide anions [Ln(OAc)5]2- are fully asymmetric and the Ln3+ cations are 10-coordinated in the form of a distorted bicapped tetragonal antiprism. This is the first report of lanthanide ions coordinated in this fashion. For Sr2+, 9-fold coordination through oxygen atoms in the form of a strongly distorted tricapped trigonal prism is observed. Furthermore, the crystallization of anhydrous, homoleptic, anionic acetate complexes from such a large variety of different metal salts appears to be due to the properties of dialkylimidazolium acetate ILs themselves, including enhanced basicity from the high concentration of free anions and their greater affinity for hydrogen-bonding solutes relative to metal cations.},
doi = {10.1021/acs.inorgchem.9b03077},
journal = {Inorganic Chemistry},
number = 1,
volume = 59,
place = {United States},
year = {2019},
month = {12}
}

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    The presence of mixed-valent silver in the uranyl phenylenediphosphonate framework
    journal, January 2020

    • Bai, Ru; Chen, Lanhua; Zhang, Yugang
    • New Journal of Chemistry, Vol. 44, Issue 15
    • DOI: 10.1039/d0nj00573h