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Hyun, S.P.; Fox, Patricia M.; Davis, James A.; Campbell, Kate M.; Hayes, Kim F.; Long, Philip E.
Pacific Northwest National Lab., Richland, WA (United States). Funding organisation: US Department of Energy (United States)2009
Pacific Northwest National Lab., Richland, WA (United States). Funding organisation: US Department of Energy (United States)2009
AbstractAbstract
[en] U(VI) adsorption by two aquifer sediment samples was studied under oxic conditions as a function of pH, U(VI), Ca, and dissolved carbonate concentration. Background-A (BKG-A) sediment was collected upstream of a former uranium mill-tailings site at Rifle, Colorado, and Little Rusty Composite (LRC) was collected on site but with low U contamination. Batch adsorption experiments were performed using artificial groundwater solutions prepared to simulate the field groundwater composition in equilibrium with specific partial pressures of carbon dioxide. To encompass the geochemical conditions of the alluvial aquifer at the site, the experimental conditions ranged from 6.8 x 10-8 to 10-5 M in [U(VI)]tot, 7.2 to 8.0 in pH, 3.0 x 10-3 to 6.0 x 10-3 M in [Ca2+], and 0.05 to 2.6% in partial pressure of carbon dioxide. The sediment was extracted with a dilute bicarbonate/carbonate solution to determine the background labile U(VI) already present in the sediment. A semi-empirical surface complexation model was developed to describe U(VI) adsorption using FITEQL4. The non-electrostatic, generalized composite surface complexation model successfully simulated U(VI) adsorption over the range of groundwater conditions at the Old Rifle site, using a two-site, two-reaction fitting scheme. The sensitivity of model parameters to background U(VI) concentration on the two samples was evaluated. U(VI) adsorption experiments were also performed using a sand fraction of BKG-A separated through repeated sonication and wet-sieving. Surface area normalized Kd for the bulk and sand fraction indicated similar reactivity for both. The surface complexation model developed in this work is expected to contribute to the prediction of fate and transport of U(VI) in the alluvial aquifer at the Old Rifle site, and to assist in the simulation of biostimulation field experiments performed at the site.
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Source
PNNL-SA--68768; KP1702030; AC05-76RL01830
Record Type
Journal Article
Journal
Environmental Science and Technology; ISSN 0013-936X; ; v. 43(24); p. 9368-9373
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