A new approach to the measurement of solubilities in supercritical CO2 is reported, utilizing laser-induced fluorescence. This selective technique was found to be capable of rapid multipoint solubility measurements with high sensitivity (10(-9) M). The sensitivity enables measurements to be performed with small amounts of analytes and at low pressure, 80-130 atm, typically below the range of other methods. Four uranyl complexes were investigated using this method, UO2(TTA)2.H20, UO2(TTA)2.TBP, UO2(TTA)2.TOPO, and UO2(NO3)2.2TBP (where TTA = thenoyltrifluoroacetone, TBP = tributyl phosphate, and TOPO = trioctyl phosphine oxide). Comparison with solubility data previously obtained with UV-visible spectroscopy shows good agreement between the techniques. We have shown that the Chrastil solubility equation is equally valid at lower ScF densities, and consequently, solubility values determined at high pressures can be extrapolated to the low-pressure regions and vice versa for solid materials.
In order to recycle potentially valuable uranium and plutonium, the Purex process has been successfully used to reprocess spent nuclear fuel for several decades now at industrial scales. The process has developed over this period to treat higher burnup fuels, oxide as well as metal
fuels within fewer solvent extraction cycles with reduced waste arisings. Within the context of advanced fuel cycle scenarios, there has been renewed international interest recently in separation technologies for recovering actinides from spent fuel. Aqueous fuel processing research and development
has included further enhancement of the Purex process as well as the development of minor actinide partitioning technologies that use new extractants. The use of single cycle Purex solvent extraction flowsheets and centrifugal contactors are key objectives in the development of such advanced
Purex processes in future closed fuel cycles. These advances lead to intensified processes, reducing the costs of plants and the volumes of wastes arising. By adopting other flowsheet changes, such as reduced fission product decontamination factors, U/Pu co-processing and Pu/Np co-stripping,
further improvements can be made addressing issues such as proliferation resistance and minor actinide burning, without adverse effects on the products. One interesting development is the demonstration that simple hydroxamic acid complexants can very effectively separate U from Np and Pu in
such advanced Purex flowsheets.
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