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Issue 23, 2012
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A highly efficient solvent system containing functionalized diglycolamides and an ionic liquid for americium recovery from radioactive wastes

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Abstract

Three room temperature ionic liquids (RTILs), viz. C4mim+·PF6, C6mim+·PF6 and C8mim+·PF6, were evaluated as diluents for the extraction of Am(III) by N,N,N′,N′-tetraoctyl diglycolamide (TODGA). At 3 M HNO3, the DAm-values by 0.01 M TODGA were found to be 102, 34 and 74 for C4mim+·PF6, C6mim+·PF6 and C8mim+·PF6, respectively. The extraction of Am(III) decreased with increasing feed acidity for all three diluents, indicating an ion exchange mechanism for the extraction. The stoichiometry of the extracted species suggested that two TODGA molecules were associated with Am(III) during the extraction for all three RTILs and the conditional extraction constants have been determined. The DM-values for different metal ions followed the order: 75 (Am(III)) > 30.7 (Pu(IV)) > 3.9 (Np(IV)) > 1.19 (Pu(VI)) > 0.52 (U(VI)) > 0.12 (Cs(I)) > 0.024 (Sr(II)). The distribution behaviour of Am(III) was also studied with a recently synthesized calix[4]arene-4DGA (C4DGA) extractant dissolved in C8mim+·PF6. Using this extractant diluent combination, the DAm-value was 194 at 3 M HNO3 using 5 × 10−5 M C4DGA, suggesting a very high distribution coefficient at very low extractant concentrations. The stoichiometry of the extracted species containing Am was found to be 1 : 2 (M : L) in C8mim+·PF6. The thermodynamics of the extraction was also studied for both extractants in C8mim+·PF6. The use of RTILs gives rise to significantly improved extraction properties than the commonly used n-dodecane and an unusual increase in separation factor values was seen for the first time which can lead to selective separation of Am from wastes containing a mixture of U, Pu and Am.

Graphical abstract: A highly efficient solvent system containing functionalized diglycolamides and an ionic liquid for americium recovery from radioactive wastes

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Publication details

The article was received on 07 Dec 2011, accepted on 23 Mar 2012 and first published on 25 Apr 2012


Article type: Paper
DOI: 10.1039/C2DT12364A
Citation: Dalton Trans., 2012,41, 6970-6979
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    A highly efficient solvent system containing functionalized diglycolamides and an ionic liquid for americium recovery from radioactive wastes

    A. Sengupta, P. K. Mohapatra, M. Iqbal, J. Huskens and W. Verboom, Dalton Trans., 2012, 41, 6970
    DOI: 10.1039/C2DT12364A

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