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

Sauerwein Fynn S.,Sittel Thomas,Geist Andreas,Panak Petra J.,Wilden Andreas,Modolo Giuseppe

EPJ Web of Conferences（2025）

Karlsruhe Institute of Technology (KIT)

Cited 0|Views4

Abstract

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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【要点】：本文研究了三价锕系元素与SO3-Ph-BTBP的络合作用，揭示了重镧系元素和钇的异常萃取行为，并提出了动力学效应是其主要原因。

【方法】：通过核磁共振（NMR）光谱学和溶剂萃取技术研究了SO3-Ph-BTBP与重镧系元素和钇的络合作用。

【实验】：实验在10^-3 mol L^-1, 1 mol L^-1 和 3 mol L^-1 DNO3溶液中进行，使用NMR光谱学证实了Lu(III)与SO3-Ph-BTBP形成了相同的络合物，并通过溶剂萃取动力学研究表明重镧系元素和钇的萃取速率缓慢，特别是在高HNO3浓度下更为显著。同时，测试了单甲基化和二甲基化TODGA衍生物与SO3-Ph-BTBP组合的性能。