Home Physical Sciences Thermodynamic model for the solubility of PuO2(am) in the aqueous Na+-H+-OH--Cl--H2O-ethylenediaminetetraacetate system
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Thermodynamic model for the solubility of PuO2(am) in the aqueous Na+-H+-OH--Cl--H2O-ethylenediaminetetraacetate system

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Published/Copyright: September 25, 2009

The solubility of PuO2(am) was determined in the aqueous Na+ H+-OH--Cl--H2O-ethylenediaminetetraacetate (EDTA) system as a function of pH (1 to 13.5) and EDTA concentrations (0.00001 to 0.093 M) to determine PuEDTA complexes important in a wide range of pH values and EDTA concentrations. The solubility studies were carried out as a function of time and show, as expected, that steady-state/equilibrium in this system is reached rapidly (<7 days). The aqueous Pu oxidation states were determined by X-ray absorption near edge spectroscopy and solvent extraction. The aqueous Pu(IV) concentrations in equilibrium with PuO2(am) at fixed concentrations of EDTA (0.0001 or 0.001;M) as a function of pH, and at fixed pH (∼9), and as a function of EDTA were interpreted using the Pitzer ion-interaction model. The model was developed based on a subset of the experimental data and was validated against the remaining, more extensive data not used in model development. The log K0 values for the formation of Pu(OH)xEDTAx- according to the generalized reaction (Pu4+ + xOH+EDTA4- ↔ Pu(OH)xEDTA-x) were determined to be 36.44±0.35, 44.78±0.35, and 49.80±0.35 for x=1, 2, and 3, respectively, when log;K0 of -56.85 for (PuO2(am)+2H2O harr; Pu4++4OH-) is used.

Published Online: 2009-9-25
Published in Print: 2001-2-1

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