SELECTIVE AMERICIUM SEPARATION: NEW INSIGHTS INTO THE COMPLEXATION OF TRIVALENT f-ELEMENTS WITH SO3-PH-BTBP

被引:0
|
作者
Sauerwein, Fynn S. [1 ]
Sittel, Thomas [2 ]
Geist, Andreas [2 ]
Panak, Petra J. [2 ,3 ]
Wilden, Andreas [1 ]
Modolo, Giuseppe [1 ]
机构
[1] Forschungszentrum Julich GmbH, Inst Fus Energy & Nucl Waste Management Nucl Wast, D-52428 Julich, Germany
[2] Karlsruhe Inst Technol KIT, Inst Nucl Waste Disposal INE, D-76021 Karlsruhe, Germany
[3] Heidelberg Univ, Inst Phys Chem, Neuenheimer Feld 253, D-69120 Heidelberg, Germany
关键词
IONIC-RADII; SOLVENT-EXTRACTION; DIGLYCOLAMIDES; LANTHANIDES; ACTINIDES; WATER;
D O I
10.1051/epjconf/202531701012
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
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 mono- and 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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页数:7
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