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Actinide-aminopolycarboxylate complexation thermodynamics: americium, berkelium, californium, and einsteinium
Urban, Matthew
Urban, Matthew
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2017
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2018-03-08
Abstract
Previous experiments revealed evidence for modestly selective interactions, encouraged by orbital degeneracy driven covalency, between berkelium and curium using the aromatic aminopolycarboxylate dipicolinic acid. To further probe the ability for the heaviest available actinides to participate in orbital degeneracy driven covalent interactions, solvent extraction competition investigations were completed with the late actinides americium, berkelium, californium, and einsteinium. These studies were completed with aliphatic aminopolycarboxylates (nitrilotriacetic acid, 2-hydroxyethyl ethylenediaminetriacetic acid, trans-1,2-cyclohexanediaminetetraacetic acid, and diethylenetriaminepentaacetic acid). The stability constants and thermodynamic parameters derived from these studies may provide some indication of covalency in heavy actinide-aliphatic amine complexation chemistry. The stability constants derived for all metal-ligand complexes in this study were compared to lanthanide stability constants of the same aminopolycarboxylates (APCs) in linear free energy relationships to address, in part, whether a difference in selectivity exists between the late actinides and their lanthanide counterparts. Californium and einsteinium displayed a 2% difference in selectivity from europium and gadolinium, respectively, in absolute terms. Little evidence was obtained that shows intra-actinide selectivity between the aliphatic amines and the trivalent actinides.
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