Abstract
Efficient separation of minor actinides and lanthanides from used nuclear fuel could potentially lead to the development of sustainable nuclear fuel cycles. Herein, we report an in-depth study on selectivity and speciation in the extraction of the trivalent minor actinide Am and rare earth metal ions with a pre-organized phenanthroline-based ligand in a hydrocarbon solvent system relevant to nuclear fuel reprocessing. The 1 : 1 and 2 : 1 ligand-to-metal complexes dominate the speciation in the organic solvent over a range of ligand-to-metal concentrations, as evidenced by experimental data and supported by modeling.
Highlights
The minor actinides (MA) americium, curium, and neptunium have high radiotoxicities and americium is the main heat contributor present in used nuclear fuel a er the ssion products 137Cs and 90Sr have decayed in the rst 300 years
The introduction of a 2octyldecyl group on the two lactam nitrogens resulted in ligand 2, shown in Fig. 1, which in comparison to bis-lactam-1,10phenanthroline ligand with n-hexyl substituents (1),[7] showed markedly improved solubility in organic solvents.[11]
To prevent the precipitation, while reaching an adequate ligand solvation within the range of ligand concentrations feasible for extraction, and to attain the most efficient separation of f-block metal ions, Isopar L with 10 vol% of Exxal 13 was chosen as the optimal organic medium for the evaluation of ligand 2 complexation with 241Am(III) and
Summary
The minor actinides (MA) americium, curium, and neptunium have high radiotoxicities and americium is the main heat contributor present in used nuclear fuel a er the ssion products 137Cs and 90Sr have decayed in the rst 300 years. This, in turn, resulted in complete extraction of both Am and Eu from aqueous solution due to abnormally high binding affinity of this ligand, hampering the elucidation of both selectivity and speciation in the organic phase.
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