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Time-Resolved Laser Fluorescence Spectroscopy and Extended X-Ray Absorption Spectroscopy Investigations of the N3- Complexation of Eu(III), Cm(III), and Am(III) in an Ionic Liquid: Differences and Similarities

Abstract : The complexation of the lanthanide Eu(III) and the actinides Cm(III) and Am(III) by N-3(-) was investigated by application of time-resolved laser fluorescence spectroscopy (TRLFS) and X-ray absorption spectroscopy (XAFS) in the ionic liquid solution Of C(4)mimTf(2)N (1-butyl-3-methylimidazolium-bis(trifluoromethylsulfonyl)imide). TRLFS, measurements show that the interaction of azide with Eu(CF3SO3)(3) and Eu(ClO4)(3) results in both dynamic luminescence quenching by collisional encounters of N-3(-) with Eu(III) and static luminescence quenching by inner-sphere complexation of Eu(III) by N-3(-). Hereby, the complexation of Eu-triflate by azide starts at a lower N-3(-) concentration as compared to the perchlorate salt. The authors ascribe this phenomenon to a stronger bonding Of ClO4- toward the metal ion than triflate, as well as to a stronger electrostatic repulsion of N-3(-) by the perchlorate ligand. In both actinide samples (Cm(ClO4)(3), Am(ClO4)(3)), the complexation with azide exhibits a clear kinetic hindrance. Nevertheless, mixed actinide-perchlorate-azide complexes are formed after several days in C(4)mimTf(2)N. The different reaction kinetics for the Ln- and An-complexation by azide may provide the opportunity for an effective separation of lanthanides from actinides in the nuclear fuel cycle by the use of N-based extractants in ionic liquid solution
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http://hal.in2p3.fr/in2p3-00289593
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Submitted on : Monday, June 23, 2008 - 9:12:53 AM
Last modification on : Monday, November 23, 2020 - 6:30:04 PM

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S. Stumpf, I. Billard, C. Gaillard, P.J. Panak, K. Dardenne. Time-Resolved Laser Fluorescence Spectroscopy and Extended X-Ray Absorption Spectroscopy Investigations of the N3- Complexation of Eu(III), Cm(III), and Am(III) in an Ionic Liquid: Differences and Similarities. Inorganic Chemistry, American Chemical Society, 2008, 47, pp.4618-4626. ⟨10.1021/ic7023567⟩. ⟨in2p3-00289593⟩

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