Spectrophotometric analysis of ternary uranyl systems to replace tri-N-butyl phosphate (TBP) in used fuel reprocessing

Canner, A. J., Harwood, L. M. ORCID: https://orcid.org/0000-0002-8442-7380, Cowell, J., Babra, J. S., Brown, S. F. and Ogden, M. D. (2020) Spectrophotometric analysis of ternary uranyl systems to replace tri-N-butyl phosphate (TBP) in used fuel reprocessing. Journal of Solution Chemistry, 49 (1). pp. 52-67. ISSN 0095-9782 doi: 10.1007/s10953-019-00942-7

Abstract/Summary

In this report, the interaction of monoamide/diamide and monoamide/diglycolamide mixtures with UO2+2 are investigated in pH = 1 methanolic nitric acid media. These monoamides include N,N-dimethylacetamide (DMAA), N,N-diethylacetamide (DEAA), N,N-dibutylacetamide (DBAA) and N,N-dibutylbutanamide (DBBA). N,N,N′N′-tetraethylmalonamide (TEMA) and N,N,N′,N′-tetraethyldiglycolamide (TEDGA), which were chosen as model diamides and diglycolamides, respectively. Complex stability constants for each ligand were modelled using the Stability Quotients Using Absorbance Data program using UV–visible data. Complex stoichiometry of ligand mixtures was determined using Job plots and UV–Vis spectrometry. Monoamides were confirmed to produce only disolvate complexes with UO2+2 in solution. The log10(K) values for monoamides were found to be independent of amine-side chain length, but were slightly dependent on the carbonyl-side chain length. TEDGA was found to produce multiple uranyl complexes in solution. Job plot data indicated that the uranyl cation strongly prefers to bond either only with the monoamide or diamide in ternary monoamide–diamide–UO2 systems. Monoamide–diglycolamide–UO2 systems were more complicated, with Job plot data indicating the potential for multiple ternary species being present is dependent on the monoamide structure.

Item Type	Article
URI	https://centaur.reading.ac.uk/id/eprint/89518
Identification Number/DOI	10.1007/s10953-019-00942-7
Refereed	Yes
Divisions	Life Sciences > School of Chemistry, Food and Pharmacy > Department of Chemistry
Publisher	Springer
Download/View statistics	View download statistics for this item