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The solubility of different forms of precipitated  242 PuO 2 (am) were examined in solutions containing aqueous Fe(II) over a range of pH values. The first series of  242 PuO 2 (am) suspensions were prepared from a  242 Pu(IV) stock that had been treated with thenoyltrifluoroacetone (TTA) to remove the  241 Am originating from the decay of  241 Pu. These  242 PuO 2 (am) suspensions showed much higher solubilities at the same pH value and Fe(II) concentration than previous studies using  239 PuO 2 (am). X-ray absorption fine structure (XAFS) spectroscopy of the precipitates showed a substantially reduced Pu–Pu backscatter over that previously observed in  239 PuO 2 (am) precipitates, indicating that the  242 PuO 2 (am) precipitates purified using TTA lacked the long range order previously found in 239 PuO 2 (am) precipitates. The Pu(IV) stock solution was subsequently repurified using an ion exchange resin and an additional series of  242 PuO 2 (am) precipitates prepared. These suspensions showed higher redox potentials and total aqueous Pu concentrations than the TTA purified stock solution. The higher redox potential and aqueous Pu concentrations were in general agreement with previous studies on  242 PuO 2 (am) precipitates, presumably due to the removal of possible organic compounds originally present in the TTA purified stock.  242 PuO 2 (am) suspensions prepared with both stock solutions showed almost identical solubilities in Fe(II) containing solutions even though the initial aqueous Pu concentrations before the addition of Fe(II) were orders of magnitude different. By examining the solubility of  242 PuO 2 (am) prepared from both stocks in this way we have essentially approached equilibrium from both the undersaturated and oversaturated conditions. The final aqueous Pu concentrations are predictable using a chemical equilibrium model which includes the formation of a nanometer sized Fe(III) reaction product, identified in the  242 PuO 2 (am) suspension both by use of  57 Fe Mössbauer spectroscopy and transmission electron microscopy (TEM) analysis.

The solubility of 242 PuO 2 in the presence of aqueous Fe(II): the impact of precipitate preparation