Chemical speciation and adsorption behavior of plutonium in natural waters
Dissolved Pu profiles in two partially anoxic basins--Saanich Inlet, an intermittently anoxic marine fiord in Vancouver Island, British Columbia, and Soap Lake, a saline, alkaline lake in eastern Washington state, revealed minimum concentrations at the O/sub 2//H/sub 2/S interface. The Pu concentrations in the anoxic waters of Saanich Inlet were less than the surface concentrations; however, in Soap Lake, a 15- to 50-fold increase in Pu concentration in the anoxic monimolimnion correlated with large increases in the major ions, total alkalinity, and dissolved organic carbon. Laboratory experiments were designed to investigate the effects of pH, ionic strength, dissolved organic carbon, and carbonate ions on the adsorption of tracer amounts of Pu IV and Pu V. The Pu-goethite adsorption system provided the data base for developing a thermodynamic model of Pu interaction with an oxide surface and with dissolved ligands, using the MINEQL computer program. Pu IV and Pu V interacted very differently with goethite, which is consistent with their different hydrolytic character. A reduction of Pu V to Pu IV occurred on the goethite surface and also on montmorillonite and silica gel, suggesting that redox transformations are an important aspect of Pu adsorption. Increases in ionic strength (up to 3 M NaCl or NaNO/sub 3/) did not affect Pu IV or 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 only 30% in the presence of 240 ppm of natural DOC from Soap Lake; however, carbonate anions inhibited Pu IV adsorption on goethite at the alkalinity levels (1500 meq/L total alkalinity, 0.57 M CO/sub 3/=) measured for Soap Lake monimolimnion waters.
- OSTI ID:
- 6866855
- Resource Relation:
- Other Information: Thesis (Ph.D.)
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
BRITISH COLUMBIA
FIORDS
ANOXIA
WATER CHEMISTRY
LAKES
PLUTONIUM
ADSORPTION
GEOCHEMISTRY
WASHINGTON
IONIC COMPOSITION
MATHEMATICAL MODELS
RADIOISOTOPES
REDOX REACTIONS
TRACER TECHNIQUES
VALENCE
ACTINIDES
CANADA
CHEMICAL REACTIONS
CHEMISTRY
ELEMENTS
ESTUARIES
FEDERAL REGION X
ISOTOPE APPLICATIONS
ISOTOPES
METALS
NORTH AMERICA
SORPTION
SURFACE WATERS
TRANSURANIUM ELEMENTS
USA
520301* - Environment
Aquatic- Radioactive Materials Monitoring & Transport- Water- (1987)