Abstract:RHO-REST -1 P WER Effects of H anford High-Level ft W aste Com ponents on Sorption o f Cobalt, S tro ntium , N eptunium , Plutonium , and A m ericium on H anford Sedim ents
“…Most ligands are also chemically unstable and are continually being transformed into molecules with even weaker complex- ' forming capabilities. Delegard and Gallagher (1983) show in an empirical fashion that relatively high concentrations of chelating agents [HEDTA to 0.1 My EDTA to 0.05 My hydroxyacetate to 0.1 M, and citrate to 0.03 MI did not increase the solubility of plutonium in tank environments. Toste et al (1984Toste et al ( ,1987) discuss procedures to analyze for specific chelatinglcomplexing agents in complex waste streams.…”
Section: 25mentioning
confidence: 86%
“…(1993), Hobbs andEdwards (1993), Hobbs (1995), Delegard et a1. (1984), Delegard and Gallagher (1983), and Delegard (1 995). However, in a recent study involving waste supernatants, Hobbs and KarrakeP) identified PuO,*XH,O in the.…”
Section: Precipitation Of Plutonium Hydroxide Phasementioning
“…Most ligands are also chemically unstable and are continually being transformed into molecules with even weaker complex- ' forming capabilities. Delegard and Gallagher (1983) show in an empirical fashion that relatively high concentrations of chelating agents [HEDTA to 0.1 My EDTA to 0.05 My hydroxyacetate to 0.1 M, and citrate to 0.03 MI did not increase the solubility of plutonium in tank environments. Toste et al (1984Toste et al ( ,1987) discuss procedures to analyze for specific chelatinglcomplexing agents in complex waste streams.…”
Section: 25mentioning
confidence: 86%
“…(1993), Hobbs andEdwards (1993), Hobbs (1995), Delegard et a1. (1984), Delegard and Gallagher (1983), and Delegard (1 995). However, in a recent study involving waste supernatants, Hobbs and KarrakeP) identified PuO,*XH,O in the.…”
Section: Precipitation Of Plutonium Hydroxide Phasementioning
“…[3,4] To address these issues, a filtration study was performed using the sixth set of samples equilibrated at 25 C to determine if submicron, actinide-containing particles in the filtered solutions contributed to the data scatter and the elevated Am solubilities. The sample preparation was performed by removing a 4-5 mL aliquot of salt solution from a sample bottle using a disposable syringe and expelling through a 0.45 μm disk filter into a clean glass vial.…”
Section: Filtration Studymentioning
confidence: 99%
“…[2] The practical usefulness of the model is limited since other constituents in the waste solution can change the Pu solubility by as much as three orders of magnitude for a given hydroxide concentration. Americium solubility in SRS waste solutions has never been systematically studied; however, there is limited data available for Hanford tank waste [3] and in pure sodium hydroxide solutions. [4] The objective of this work was to measure the solubility of Pu and Am in simulated SRS waste solutions over a broader range of solution compositions and temperature.…”
Section: Introductionmentioning
confidence: 99%
“…[3,4] For this reason, a filtration study was performed to determine if submicron, actinide-containing particles in the filtered solutions contributed to the data scatter and the elevated Am solubilities. Results from this study showed that Am particles were not completely removed during sample preparation and, thus, the Am data were not suitable for determining the Am solubility.…”
To address the accelerated disposition of the supernate and salt portions of Savannah River Site (SRS) high level waste (HLW), solubility experiments were performed to develop a predictive capability for plutonium (Pu) solubility. A statistically designed experiment was used to measure the solubility of Pu in simulated solutions with salt concentrations and temperatures which bounded those observed in SRS HLW solutions. Constituents of the simulated waste solutions included: hydroxide (OH No discernable time dependence of the measured Pu concentrations was observed except for two salt solutions equilibrated at 80 C which contained OH -concentrations > 5 mol/L. In these solutions, the Pu solubility increased with time. This observation was attributed to the air oxidation of a portion of the Pu from Pu(IV) to the more soluble Pu(V) or Pu(VI) valence states. A data driven approach was subsequently used to develop a modified response surface model for Pu solubility. Solubility data from this study and historical data from the literature were used to fit the model. The model predicted the Pu solubility of the solutions from this study within the 95% confidence interval for individual predictions and the analysis of variance indicated no statistically significant lack of fit.The Savannah River National Laboratory (SRNL) model was compared with predicted values from the Aqueous Electrolyte (AQ) model developed by OLI Systems, Inc. and a solubility prediction equation developed by Delegard and Gallagher for Hanford tank waste. The agreement between measured or values predicted by the SRNL model and values predicted by the OLI AG model was very poor. The much higher predicted concentrations by the OLI AQ model appears to be the result of the model predicting the predominate Pu oxidation state is Pu(V) which is reported as unstable below sodium hydroxide (NaOH) concentrations of 6 M. There was very good agreement between the predicted Pu concentrations using the SRNL model and the model developed by Delegard and Gallagher with the exception of solutions that had very high OH -(15 M) concentrations. The lower Pu solubilities in these solutions were attributed to the presence of NO 3 -and NO 2
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