SOLVENT EXTRACTION SEPARATION OF TRIVALENT AMERICIUM FROM CURIUM AND THE LANTHANIDES

被引:34
|
作者
Jensen, Mark P. [1 ]
Chiarizia, Renato [1 ]
Ulicki, Joseph S. [2 ]
Spindler, Brian D. [2 ]
Murphy, Daniel J. [2 ]
Hossain, M. Mahmun [2 ]
Roca-Sabio, Adrian [3 ]
de Blas, Andres [3 ]
Rodriguez-Blas, Teresa [3 ]
机构
[1] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA
[2] Univ Wisconsin, Dept Chem & Biochem, Milwaukee, WI 53201 USA
[3] Univ A Coruna, Dept Quim Fundamental, Coruna, Spain
关键词
americium; curium; actinide-lanthanide separation; crown-ether; COMPLEXES; ACTINIDES; ACID; OXIDATION; KINETICS; DISSOCIATION; STABILITY; MECHANISM; AM(III); CM(III);
D O I
10.1080/07366299.2015.1046292
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The sterically constrained, macrocyclic, aqueous soluble ligand N,N-bis[(6-carboxy-2-pyridyl)methyl]-1,10-diaza-18-crown-6 (H(2)BP18C6) was investigated for separating americium from curium and all the lanthanides by solvent extraction. Pairing H(2)BP18C6, which favors complexation of larger f-element cations, with acidic organophosphorus extractants that favor extraction of smaller f-element cations, such as bis-(2-ethylhexyl)phosphoric acid (HDEHP) or (2-ethylhexyl)phosphonic acid mono(2-ethylhexyl) ester (HEH[EHP]), created solvent extraction systems with good Cm/Am selectivity, excellent trans-lanthanide selectivity (K-ex,K-Lu/K-ex,K-La = 10(8)), but poor selectivity for Am against the lightest lanthanides. However, using an organic phase containing both a neutral extractant, N,N,N',N'-tetra(2-ethylhexyl)diglycolamide (TEHDGA), and HEH[EHP] enabled rejection of the lightest lanthanides during loading of the organic phase from aqueous nitric acid, eliminating their interference in the americium stripping stages. In addition, although it is a macrocyclic ligand, H(2)BP18C6 does not significantly impede the mass transfer kinetics of the HDEHP solvent extraction system.
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页码:329 / 345
页数:17
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