The effect of phosphate treatment on lead relative bioavailability (Pb RBA) was assessed in three distinct Pb-contaminated soils. Phosphoric acid (PA) or rock phosphate were added to smelter (PP2), nonferrous slag (SH15), and shooting range (SR01) impacted soils at a P:Pb molar ratio of 5:1. In all of the phosphate amended soils, Pb RBA decreased compared to that in untreated soils when assessed using an in vivo mouse model. Treatment effect ratios (i.e., the ratio of Pb RBA in treated soil divided by Pb RBA in untreated soil) ranged from 0.39 to 0.67, 0.48 to 0.90, and 0.03 to 0.19 for PP2, SH15, and SR01, respectively. The decrease in Pb RBA following phosphate amendment was attributed to the formation of poorly soluble Pb phosphates (i.e., chloropyromorphite, hydroxypyromorphite, and Pb phosphate) that were identified by X-ray absorption spectroscopy (XAS). However, a similar decrease in Pb RBA was also observed in untreated soils following the sequential gavage of phosphate amendments. This suggests that in vivo processes may also facilitate the formation of poorly soluble Pb phosphates, which decreases Pb absorption. Furthermore, XAS analysis of PA-treated PP2 indicated further in vivo changes in Pb speciation as it moved through the gastrointestinal tract, which resulted in the transformation of hydroxypyromorphite to chloropyromorphite.

A number of bioaccessibility methodologies have the potential to act as surrogate measures of arsenic (As) relative bioavailability (RBA), however, validation of the in vivo-in vitro relationship is yet to be established. Validation is important for human health risk assessment in order to ensure robust models for predicting As RBA for refining exposure via incidental soil ingestion. In this study, 13 As-contaminated soils were assessed for As RBA (in vivo swine model) and As bioaccessibility (Solubility Bioaccessibility Research Consortium gastric phase extraction; SBRC-G). In vivo and in vitro data were used to assess the validity of the As RBA-bioaccessibility correlation previously described by Juhasz et al. (2009). Arsenic RBA and bioaccessibility in the 13 soils ranged from 6.8±2.4% to 70.5±6.8% and 5.7±0.3% to 78.4±0.8% respectively with a strong linear relationship (R2=0.75) between in vivo and in vitro assays. When the As in vivo-in vitro correlation was compared that of Juhasz et al. (2009), there was no significant difference (P>0.05) indicating that the relationship between As RBA and As bioaccessibility was consistent thereby demonstrating its validation. For these data, a grouped linear regression model was developed (R2=0.82) with a slope and y-intercept of 0.84 and 3.56 respectively. A number of cross validation methodologies (2-fold, repeat random subsampling, leave one out) were utilized to determine the performance of the linear regression model. Residuals and prediction errors ranged from 5.4 to 9.4 and 6.9-12.2 respectively illustrating the capacity of the SBRC-G to accurately predict As RBA in contaminated soil.

In this study, previously established arsenic (As) in vivo-in vitro correlations (IVIVC) were assessed for their validity using an independent data set comprising As relative bioavailability (RBA) and bioaccessibility values for 13 herbicide- and mine-impacted soils. The validation process established the correlation between As RBA (swine model) and bioaccessibility (five in vitro assays), determined whether correlations differed significantly from previous relationships and assessed model bias and error. The capacity of in vitro assays to predict As RBA was demonstrated by the strength of IVIVC; goodness of fit ranged from 0.53 (DIN-I) to 0.74 (UBM-I). When compared to previous IVIVC (Juhasz et al. Environ. Sci. Technol. 2009 , 43 , 9487 ; Juhasz et al. J. Hazard. Mater. 2011 , 197 , 161 ), there was no significant difference (P < 0.01) in the slope and y-intercept for IVG-G, UBM-G, and UBM-I indicating the consistency of these assays for predicting As RBA. However, variability in model bias and prediction error was observed with significantly lower (P < 0.01) error determined for IVG-G suggesting that As RBA predictions using IVG-G may be more robust compared to UBM-G and UBM-I. In contrast, differences in the slope and/or y-intercept were observed for SBRC-I, IVG-I, PBET-G, PBET-I, DIN-G, and DIN-I suggesting that these methodologies may not be suitable for predicting As RBA.

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