Exposure to mercury (Hg)-contaminated soils may pose a health risk to children by way of oral, dermal, and inhalatory pathways. However, risk characterization studies, including contaminant bioaccessibility with child-specific exposure parameters and scenarios, are lacking. The objectives of this study were (1) to assess children's Hg exposure using characterization and oral bioaccessibility data from Hg-contaminated soils characterized in previous studies (n = 8); and (2) to characterize probabilistic risk in terms of hazard index (HI) considering ingestion, dermal, and inhalation pathways. Total Hg concentrations in soils ranged from 2.61 to 1.15 × 10(4) mg kg(-1). For moderately contaminated soils (S1-S5: Hg ≤ 12.15 mg kg(-1)), low oral bioaccessibility values (1.5-7.5 %) lead to HI < 1 in all scenarios. However, exposure to highly contaminated soils (S6-S8) may pose serious risks to children under normal exposure (HI 0.89-66.5) and soil-pica behaviour scenarios (HI up to 131). All three pathways significantly contributed to the risk. Using total Hg concentrations in calculations (assuming 100 % bioavailability) instead of considering Hg bioavailability leads to risk overestimation. Further research on oral, inhalatory, and dermal bioavailability of Hg, as well as child play behaviour, is recommended to obtain more accurate risk estimates.
Ingestion of contaminated soils by children during hand-to-mouth activities can be a significant exposure pathway to toxic chemicals. Bioaccessibility, which corresponds to the fraction of an ingested contaminant dissolved in the gastrointestinal tract and potentially available for absorption, can be determined by in vitro extractions and gives a conservative value of relative oral bioavailability. The goal of this study was to investigate the validity of the CDM in vitro extraction protocol, developed by Camp Dresser and Mc Kee, by assessing the influence of soil properties and Hg fractionation on bioaccessibility. Mercury bioaccessibility was determined in two pure mercury compounds, two reference materials (a soil and a sediment), and three field-collected contaminated soils. Soils and reference materials were characterized and a sequential extraction procedure was applied to the samples. Bioaccessibility of HgCl(2) was 99.8% in the gastric phase and 88.6% in the intestinal phase, whereas bioaccessibility of HgS was lower than 0.01%. In field-collected soils A, B, M, and, in ERM-CC580, mercury bioaccessibility was lower than 3.2% (below detection). In contrast, CRM 025-050 had a high Hg bioaccessibility (44.3% for gastric phase and 34.7% for intestinal phase). Gastric and intestinal bioaccessibility values were positively correlated with sulfate content in soils (r = 0.99, p < 0.001, for both gastric and intestinal bioaccessibility). In field-collected soils and ERM-CC580, the residual fraction represented near 100% of the mercury recovered, with less than 2% of mercury being in the water-soluble (F1) and CaCl(2)-exchangeable (F2) fractions. In contrast, 46% of mercury in the reference material CRM 025-050 was extracted in the CaCl(2)-exchangeable fraction. Results of the sequential extractions were in agreement with bioaccessibility values, with the sum of the water-soluble and CaCl(2)-exchangeable fractions (F1 + F2) highly correlated with intestinal bioaccessibility values (r = 0.99, p < 0.001). Hence, the sequential extraction procedure used in this study could be a simple means to help validate mercury bioaccessibility.
Soil ingestion by children can be a significant exposure pathway to mercury (Hg). Unfortunately, no reliable in vivo results for Hg oral bioavailability determination in soils have been published. In vitro extractions enable the assessment of metals' bioaccessibility, which is an estimate of oral bioavailability. Therefore, the goal of this study was to evaluate two in vitro protocols (CDM (Camp Dresser and Mc Kee Inc.) and IVG (In Vitro Gastrointestinal)) for determination of Hg bioaccessibility in soils using pure Hg-compounds, reference materials (CRM 025-050 and ERM-CC580), and field-collected soils with elevated Hg concentrations. The influence of Hg fractionation and soil properties on Hg bioaccessibility was also investigated. In the field-collected soils, IVG bioaccessibility ranged from 1.5 to 7.5%, and was always below 3.15%, using the CDM method. Mercury bioaccessibility in CRM 025-050 was 61.5 and 34.7%, using IVG and CDM protocols, respectively, whereas Hg bioaccessibility was much lower in the certified sediment sample ERM-CC580 (<7%). Overall, the CDM protocol resulted in lower Hg bioaccessibility values. The water-soluble and exchangeable Hg fraction was highly correlated with gastrointestinal bioaccessibility (r=0.99, p<0.001 for both methods) and this fraction could be a potentially good indicator of Hg bioaccessibility. Because the IVG method is less time-consuming than the CDM protocol and includes organic physiological components which seem to increase Hg bioaccessibility, it might be preferred for determination of Hg bioaccessibility.
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