001     1017129
005     20240708133958.0
037 _ _ |a FZJ-2023-03950
041 _ _ |a English
100 1 _ |a Sauerwein, Fynn Sören
|0 P:(DE-Juel1)167486
|b 0
|e Corresponding author
|u fzj
111 2 _ |a IEK-6 Institutsseminar
|c Jülich
|w Germany
245 _ _ |a Characterization of f-element complexes with soft-donorligands (f-Char)
|f 2023-10-18 -
260 _ _ |c 2023
336 7 _ |a Conference Paper
|0 33
|2 EndNote
336 7 _ |a Other
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336 7 _ |a INPROCEEDINGS
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336 7 _ |a LECTURE_SPEECH
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336 7 _ |a Talk (non-conference)
|b talk
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|s 1698125139_21860
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336 7 _ |a Other
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520 _ _ |a The German research project f-Char, funded by the German Federal Ministry of Education and Research (BMBF), contributes to a better understanding of the coordination chemistry of ac-tinide (An) and lanthanide (Ln) ions with ligands coordinating via soft donor atoms, e.g., N donor atoms. Since recycling of minor actinides from PUREX raffinate solution is a decisive step towards closing the nuclear fuel cycle, current research focuses on the challenging sepa-ration of Am(III) from Cm(III) and other trivalent fission lanthanides. The Americium Selective (AmSel) process[1] was designed for this task combining the water-soluble tetradentate N-do-nor ligand SO3-Ph-BTBP (tetrasodium-3,3',3'',3'''-([2,2'-bipyridine]-6,6'-diylbis(1,2,4-triazine-3,5,6-triyl))tetrabenzenesulfonate) with the well-known An(III)/Ln(III) coextracting agent TODGA (N,N,N',N'-tetra-n-octyl diglycolamide). While the separation of Am from Cm and the light Ln (La-Gd) is possible, a significant drop in distribution ratios of the heavy Ln (Tb-Lu) can be observed for ≥ 1 mol L-1 HNO3. This unusual behavior was further investigated looking at the complexation of SO3-Ph-BTBP with different Ln using different spectroscopic methods (UV/Vis, NMR). While SO3-Ph-BTBP complexation at low nitric acid concentration (10-3 mol L-1 HNO3) is observed for all lanthanides (Nd, Sm, Ho, Lu), complex formation at high nitric acid concentration (3 mol L-1 HNO3) is only observed for heavy Ln (Ho, Lu). Regardless of the nitric acid concentration, NMR spectra always show the same SO3-Ph-BTBP complex speciation with Ln. Interestingly, the complexation equilibrium for heavy Ln in 3 mol L-1 nitric acid solution is established very slowly (6 – 22 h). This effect was also confirmed by kinetic batch extraction studies and is presumably caused by the kinetically inhibited (de)complexation of the [Ln(SO3-Ph-BTBP)x] complexes. However, the mechanism is not yet understood and requires further studies.Furthermore, the two new N-donor ligands MTB (6-(6-methyl-1,2,4,5-tetrazin-3-yl)-2,2'-bipyr-idine) and PPTMP ((4-(6-(1,10-phenanthrolin-2-yl)pyridin-2-yl)-1H-1,2,3-triazol-1-yl)methyl pivalate) were tested as alternative extractants for the An(III)/Ln(III) separation. Both extract-ants were able to achieve good extraction efficiency into different diluents (tert-butylbenzene, toluene, nitrobenzene) at low nitric acid concentrations < 0.1 mol L-1 HNO3 and in presence of the lipophilic anion source 2-bromodecanoic acid.[1] C. Wagner et al., Solvent Extr. Ion Exch., 2016. 34 (2): p. 103-113, DOI: 10.1080/07366299.2015.1129192.
536 _ _ |a 1412 - Predisposal (POF4-141)
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536 _ _ |a Verbundprojekt f-Char: Spektroskopische Charakterisierung von f-Element-Komplexen mit soft donor-Liganden, Teilprojekt D (02NUK059D)
|0 G:(BMBF)02NUK059D
|c 02NUK059D
|x 1
700 1 _ |a Sittel, Thomas
|0 P:(DE-HGF)0
|b 1
700 1 _ |a Grieser, Fabian
|0 P:(DE-HGF)0
|b 2
700 1 _ |a Wilden, Andreas
|0 P:(DE-Juel1)130438
|b 3
|u fzj
700 1 _ |a Modolo, Giuseppe
|0 P:(DE-Juel1)130383
|b 4
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910 1 _ |a Forschungszentrum Jülich
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913 1 _ |a DE-HGF
|b Forschungsbereich Energie
|l Nukleare Entsorgung, Sicherheit und Strahlenforschung (NUSAFE II)
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914 1 _ |y 2023
920 _ _ |l yes
920 1 _ |0 I:(DE-Juel1)IEK-6-20101013
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980 _ _ |a talk
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980 _ _ |a I:(DE-Juel1)IEK-6-20101013
980 _ _ |a UNRESTRICTED
981 _ _ |a I:(DE-Juel1)IFN-2-20101013


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