Selective Americium Separation: New Insights into the Complexation of Trivalent f-Elements with SO3-Ph-BTBP

In the Americium selective (AmSEL) process, the N-donor ligand 3,3’,3’’,3’’’-([2,2’-bipyridine]-6,6’-diylbis(1,2,4-triazine-3,5,6-triyl))tetrabenzenesulfonate (SO3-Ph-BTBP) is used to selectively strip Am(III) from a N,N,N’,N’-tetraoctyl diglycolamide (TODGA) containing organic phase loaded with Am(...

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Main Authors: Sauerwein Fynn S., Sittel Thomas, Geist Andreas, Panak Petra J., Wilden Andreas, Modolo Giuseppe
Format: Article
Language:English
Published: EDP Sciences 2025-01-01
Series:EPJ Web of Conferences
Online Access:https://www.epj-conferences.org/articles/epjconf/pdf/2025/02/epjconf_atalante2025_01012.pdf
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author Sauerwein Fynn S.
Sittel Thomas
Geist Andreas
Panak Petra J.
Wilden Andreas
Modolo Giuseppe
author_facet Sauerwein Fynn S.
Sittel Thomas
Geist Andreas
Panak Petra J.
Wilden Andreas
Modolo Giuseppe
author_sort Sauerwein Fynn S.
collection DOAJ
description In the Americium selective (AmSEL) process, the N-donor ligand 3,3’,3’’,3’’’-([2,2’-bipyridine]-6,6’-diylbis(1,2,4-triazine-3,5,6-triyl))tetrabenzenesulfonate (SO3-Ph-BTBP) is used to selectively strip Am(III) from a N,N,N’,N’-tetraoctyl diglycolamide (TODGA) containing organic phase loaded with Am(III), Cm(III) and lanthanides (Ln(III)). Fundamental extraction mechanism studies revealed an unusual extraction behavior of heavy Ln(III) and Y(III), which provided the motivation to investigate their complexation with SO3-Ph-BTBP using nuclear magnetic resonance (NMR) spectroscopy and solvent extraction. NMR spectroscopy indicated the formation of the same SO3-Ph-BTBP complex with Lu(III) in 10-3 mol L-1, 1 mol L-1 and 3 mol L-1 DNO3 solution. However, the complexation at high DNO3 concentration is subject to a slower than expected complexation kinetics leading to the conclusion that the unusual extraction behavior is probably related to a kinetics effect rather than an unknown complex species. Kinetics studies using solvent extraction show a slowly increasing extraction of heavy Ln(III) and Y(III) into the organic phase which is attributed to a kinetically inhibited decomplexation of the SO3-Ph-BTBP complexes. This effect is even more pronounced at higher HNO3 concentration. Additionally, combinations of monoand di-methylated TODGA derivatives with SO3-Ph-BTBP were tested, showing a decreasing performance regarding the actinide(III)/lanthanide(III) and Am(III)/Cm(III) separation with increasing degree of methylation.
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spelling doaj-art-1e9c2e00f8314a7faaa9cd613403138d2025-02-05T10:53:04ZengEDP SciencesEPJ Web of Conferences2100-014X2025-01-013170101210.1051/epjconf/202531701012epjconf_atalante2025_01012Selective Americium Separation: New Insights into the Complexation of Trivalent f-Elements with SO3-Ph-BTBPSauerwein Fynn S.0Sittel Thomas1Geist Andreas2Panak Petra J.3Wilden Andreas4Modolo Giuseppe5Institute of Fusion Energy and Nuclear Waste Management – Nuclear Waste Management (IFN-2), Forschungszentrum Jülich GmbHKarlsruhe Institute of Technology (KIT), Institute for Nuclear Waste Disposal (INE)Karlsruhe Institute of Technology (KIT), Institute for Nuclear Waste Disposal (INE)Karlsruhe Institute of Technology (KIT), Institute for Nuclear Waste Disposal (INE)Institute of Fusion Energy and Nuclear Waste Management – Nuclear Waste Management (IFN-2), Forschungszentrum Jülich GmbHInstitute of Fusion Energy and Nuclear Waste Management – Nuclear Waste Management (IFN-2), Forschungszentrum Jülich GmbHIn the Americium selective (AmSEL) process, the N-donor ligand 3,3’,3’’,3’’’-([2,2’-bipyridine]-6,6’-diylbis(1,2,4-triazine-3,5,6-triyl))tetrabenzenesulfonate (SO3-Ph-BTBP) is used to selectively strip Am(III) from a N,N,N’,N’-tetraoctyl diglycolamide (TODGA) containing organic phase loaded with Am(III), Cm(III) and lanthanides (Ln(III)). Fundamental extraction mechanism studies revealed an unusual extraction behavior of heavy Ln(III) and Y(III), which provided the motivation to investigate their complexation with SO3-Ph-BTBP using nuclear magnetic resonance (NMR) spectroscopy and solvent extraction. NMR spectroscopy indicated the formation of the same SO3-Ph-BTBP complex with Lu(III) in 10-3 mol L-1, 1 mol L-1 and 3 mol L-1 DNO3 solution. However, the complexation at high DNO3 concentration is subject to a slower than expected complexation kinetics leading to the conclusion that the unusual extraction behavior is probably related to a kinetics effect rather than an unknown complex species. Kinetics studies using solvent extraction show a slowly increasing extraction of heavy Ln(III) and Y(III) into the organic phase which is attributed to a kinetically inhibited decomplexation of the SO3-Ph-BTBP complexes. This effect is even more pronounced at higher HNO3 concentration. Additionally, combinations of monoand di-methylated TODGA derivatives with SO3-Ph-BTBP were tested, showing a decreasing performance regarding the actinide(III)/lanthanide(III) and Am(III)/Cm(III) separation with increasing degree of methylation.https://www.epj-conferences.org/articles/epjconf/pdf/2025/02/epjconf_atalante2025_01012.pdf
spellingShingle Sauerwein Fynn S.
Sittel Thomas
Geist Andreas
Panak Petra J.
Wilden Andreas
Modolo Giuseppe
Selective Americium Separation: New Insights into the Complexation of Trivalent f-Elements with SO3-Ph-BTBP
EPJ Web of Conferences
title Selective Americium Separation: New Insights into the Complexation of Trivalent f-Elements with SO3-Ph-BTBP
title_full Selective Americium Separation: New Insights into the Complexation of Trivalent f-Elements with SO3-Ph-BTBP
title_fullStr Selective Americium Separation: New Insights into the Complexation of Trivalent f-Elements with SO3-Ph-BTBP
title_full_unstemmed Selective Americium Separation: New Insights into the Complexation of Trivalent f-Elements with SO3-Ph-BTBP
title_short Selective Americium Separation: New Insights into the Complexation of Trivalent f-Elements with SO3-Ph-BTBP
title_sort selective americium separation new insights into the complexation of trivalent f elements with so3 ph btbp
url https://www.epj-conferences.org/articles/epjconf/pdf/2025/02/epjconf_atalante2025_01012.pdf
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