Computer Science
Scientific paper
Nov 1985
adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=1985gecoa..49.2297s&link_type=abstract
Geochimica et Cosmochimica Acta, vol. 49, Issue 11, pp.2297-2307
Computer Science
4
Scientific paper
The adsorption of Pu(IV) and Pu(V) on goethite ( FeOOH) from NaNO 3 solution shows distinct differences related to the different hydrolytic character of these two oxidation states. Under similar solution conditions, the adsorption edge of the more strongly hydrolyzable Pu(IV) occurs in the pH range 3 to 5 while that for Pu(V) is at pH 5 to 7. The adsorption edge for Pu(V) shifts with time to lower pH values and this appears to be due to the reduction of Pu(V) to Pu(IV) in the presence of the goethite surface. These results suggest that redox transformations may be an important aspect of Pu adsorption chemistry and the resulting scavenging of Pu from natural waters. Increasing ionic strength (from 0.1 M to 3 M NaCl or NaNO 3 and 0.03 M to 0.3 M Na 2 SO 4 ) did not influence Pu(IV) or Pu(V) adsorption. In the presence of dissolved organic carbon (DOC), Pu(V) reduction to Pu(IV) occurred in solution. Pu(IV) adsorption on goethite decreased by 30% in the presence of 240 ppm natural DOC found in Soap Lake, Washington waters. Increasing concentrations of carbonate ligands decreased Pu(IV) and Pu(V) adsorption on goethite, with an alkalinity of 1000 meq/l totally inhibiting adsorption. The Pu-goethite adsorption system provides the data base for developing a thermodynamic model of Pu interaction with an oxide surface and with dissolved ligands, using the MINEQL computer program. From the model calculations we determined equilibrium constants for the adsorption of Pu(IV) hydrolysis species. The model was then applied to Pu adsorption in carbonate media to see how the presence of CO 3 -2 could influence the mobility of Pu. The decrease in adsorption appears to be due to formation of a Pu-CO 3 complex. Model calculations were used to predict what the adsorption curves would look like if Pu-CO 3 complexes formed.
Murray James W.
Sanchez Arthur L.
Sibley Thomas H.
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