Comparison of Approaches to Calibrate a Surface Complexation Model for U(VI) Sorption to Weathered Saprolite |
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Authors: | F Zhang J C Parker S C Brooks Y-J Kim G Tang P M Jardine D B Watson |
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Institution: | (1) Environmental Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA;(2) Department of Civil and Environmental Engineering, University of Tennessee, Knoxville, TN 37996, USA;(3) School of Civil, Urban, & Geosystem Engineering, Seoul National University, Shilim-Dong, Gwanak-Gu, Seoul, 151-744, South Korea |
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Abstract: | A surface complexation model describing the sorption of uranyl ions and uranyl carbonate on weak and strong sites was used
to analyze experiments conducted on pH-dependent U(VI) sorption to weathered shale/limestone saprolite. Sorption data were
collected at two different solid to solution ratios. Various methods of estimating equilibrium reaction coefficients and site
densities were investigated. As a first approximation, extractable iron oxides were assumed to behave as ferrihydrite with
reaction coefficients as reported by Waite (Geochim Cosmochim Acta 58:5465–5478, 1994). A generalized composite (GC) approach
was then employed with coefficients estimated by an inverse modeling method applied both in a stepwise fashion and simultaneously
to whole data set. Uncertainty in model parameters and predictions was lowest using the simultaneous inverse method, but results
from the stepwise method were very similar. The generalized reaction network accurately described pH-dependent U(VI) sorption
on weathered saprolite between pH 4 and 9. |
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Keywords: | U(VI) Sorption Saprolite Surface complexation Generalized composite method |
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