Supercritical fluid extraction of plutonium and americium from soil using thenoyltrifluoroacetone and tributylphosphate complexation

Abstract

Samples of clean soil from the source used to backfill pits at the Idaho National Engineering and Environmental Laboratory´s Radioactive Waste Management Complex were spiked with239Pu and241Am to evaluate ligand-assisted supercritical fluid extraction as a decontamination method. The actual soil in the pits has been subject to approximately three decades of weathering since it was originally contaminated. No surrogate soil can perfectly simulate the real event, but actual contaminated soil was not available for research purposes. However, fractionation of Am and Pu in the surrogate soil was found to be similar to that previously measured in the real soil using a sequential aqueous extraction procedure. This suggests that Pu and Am behavior are similar in the two soils. The surrogate was subjected to supercritical carbon dioxide extraction, in the presence of the fluorinated beta diketone thenoyltrifluoroacetone (TTA), and tributylphosphate (TBP). As much as 69% of the Pu and 88% of the Am were removed from the soil using 3.2 mol.% TTA and 2.7 mol.% TBP, in a single 45 minute extraction. Extraction conditions employing a 5 mol.% ethanol modifier with 0.33 mol.% TTA and 0.27 mol.% TBP resulted in 66% Pu and 68% Am extracted. To our knowledge, this is the first report of the use of supercritical fluid extraction (SFE) for the removal of actinides from soil.