Abstract
The role of organic matter (OM) in antimonate (further denoted as Sb(OH)6) mobility in soil is unclear. The objective of this study was to evaluate Sb(OH)6–OM interaction. Antimonate solid:liquid distribution coefficients (KD) were measured at low Sb concentrations in soil samples with a natural gradient in soil organic carbon (OC) that were collected from different depths of up to 3 m in two excavated soil profiles and in a subset of four soil samples with experimentally increased OM concentration from addition of Suwannee River OM. The KD values were related to soil properties by multiple linear regression and described with the CD–MUSIC model of ferrihydrite. The KD values ranged from 12 to 2800 L kg−1 and decreased strongly with increasing OC concentrations, when normalized to the amount of iron (Fe) and aluminium (Al) in acid oxalate extracts (r = −0.69; p < 0.0001). Experimentally increasing OC by ∼1.5 g kg−1 increased soluble Sb and decreased Sb(OH)6KD values by up to a factor of 8. The multiple regression model reveals that sorption of Sb(OH)6 to Fe and Al hydroxides decreases with increasing pH and increasing dissolved organic carbon concentration. This effect could be explained with geochemical modelling by the competitive and electrostatic effects of adsorbed humic substances on Sb(OH)6 surface complexation to the reactive surface sites of the Fe and Al hydroxides. Finally, both models could predict the in situ pore water Sb concentrations of unspiked samples, with a RMSE of 0.35 for the regression model and 0.43 for the geochemical model on the log10Sb concentrations. For these predictions, the 0.1 M Na2HPO4–extractable Sb concentration was measured and used to estimate the reversibly sorbed Sb pool. This study shows that increasing soil OM increases Sb(OH)6 mobility at low soil Sb concentration, likely due to competitive sorption on Fe and Al hydroxides and a process based, geochemical model was calibrated to describe Sb(OH)6 mobility in soil.
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