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Comparison of analytical charge-form and equilibrium thermodynamic speciation of certain radionuclides

Conference ·
OSTI ID:7008624
Calculating trace element speciation with a thermodynamic model is often challenged on the basis that the existing thermodynamic data are not sufficiently reliable. Water quality data and corresponding analytical charge-form speciation analyses were available for radionuclides occurring in a low-level radioactive groundwater. This offered a unique opportunity for comparing the results of an equilibrium thermodynamic model with the results of analytical charge-form speciation. The charge-form speciation was determined using the Battelle Large Volume Water Sampler, which contains consecutive layers of cation resin, anion resin and activated aluminum oxide for retention of cationic, anionic and non-ionic dissolved chemical species, respectively. The thermodynamic speciation of Cs, Cr, Fe, I, Mn, Mo, Na, and Zn was calculated using the MINTEQ geochemical model. Other radioactive elements (Ce, Co, Tc, Np, Pm and Sb) were speciated by hand calculation. Excellent agreement between the analytically determined charge-form and the thermodynamic speciation was observed for several radionuclides (/sup 54/Mn, /sup 144/Ce, /sup 131/I, /sup 24/Na, /sup 137/Cs, /sup 99/Mo, /sup 99/Tc, /sup 151/Pm, /sup 151/Np). Organic complexation by natural and/or synthetic organics in the waters may be important in the speciation of /sup 65/Zn, /sup 60/Co, /sup 131/I, /sup 59/Fe and possibly /sup 51/Cr. Both /sup 124/Sb and /sup 125/Sb appeared to be in redox disequilibria with the groundwater. 28 references, 2 tables.
Research Organization:
Pacific Northwest Lab., Richland, WA (USA)
DOE Contract Number:
AC06-76RL01830
OSTI ID:
7008624
Report Number(s):
PNL-SA-12093; CONF-840408-13; ON: DE84011896
Country of Publication:
United States
Language:
English

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