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The solubility of PuO 2 (am) was determined in the aqueous Na +  H + -OH - -Cl - -H 2 O-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 (&lt;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 PuO 2 (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 K 0  values for the formation of Pu(OH) x EDTA x-  according to the generalized reaction (Pu 4+  + xOH  +EDTA 4-  ↔ Pu(OH) x EDTA -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;K 0  of -56.85 for (PuO 2 (am)+2H 2 O harr; Pu 4+ +4OH - ) is used.

Thermodynamic model for the solubility of PuO 2 (am) in the aqueous Na + -H + -OH - -Cl - -H 2 O-ethylenediaminetetraacetate system