House dust and soils can be major sources of lead (Pb) exposure for children. The American Healthy Homes Survey (AHHS) was developed to estimate Pb exposure from house dust and soil, in addition to other potential household contaminants and allergens. We have combined Xray absorption spectroscopic (XAS) fingerprinting and in vivo mouse relative bioavailability (RBA) measurements for a subset of house dust and residential soils collected in the AHHS, with the primary objective of gaining a better understanding of determinants of house dust Pb bioavailability. Lead speciation was well related to variations in RBA results and revealed that highly bioavailable Pb (hydroxy)carbonate (indicative of Pb-based paint) was the major Pb species present in house dusts. Measured Pb RBA was up to 100% and is likely driven by paint Pb. To our knowledge, this is the first report of in vivo Pb RBA for U.S. house dust contaminated in situ with paint Pb and corroborates results from a previous study that demonstrated high RBA of paint Pb added to soil. We also report a relatively low RBA (23%) in a residential soil where the major Pb species was found to be plumbojarosite, consistent with a previous report that plumbojarosite lowers Pb RBA in soils.

Lead (Pb) contamination of soils is of global concern due to the devastating impacts of Pb exposure in children. Because early-life exposure to Pb has long-lasting health effects, reducing exposure in children is a critical public health goal that has intensified research on the conversion of soil Pb to low bioavailability phases. Recently, plumbojarosite (PLJ) conversion of highly available soil Pb was found to decrease Pb relative bioavailability (RBA <10%). However, there is sparse information concerning interactions between Pb and other elements when contaminated soil, pre- and post-remediation, is ingested and moves through the gastrointestinal tract (GIT). Addressing this may inform drivers of effective chemical remediation strategies. Here, we utilize bulk and micro-focused Pb X-ray absorption spectroscopy to probe elemental interactions and Pb speciation in mouse diet, cecum, and feces samples following ingestion of contaminated soils pre- and post-PLJ treatment. RBA of treated soils was less than 1% with PLJ phases transiting the GIT with little absorption. In contrast, Pb associated with organics was predominantly found in the cecum. These results are consistent with transit of insoluble PLJ to feces following ingestion. The expanded understanding of Pb interactions during GIT transit complements our knowledge of elemental interactions with Pb that occur at higher levels of biological organization.

Methods promoting lead (Pb) phase transformation in soils are essential for decreasing Pb bioaccessibility/ bioavailability and may offer an in situ, cost-efficient process for mitigating contaminant exposure. Recent plumbojarosite (PLJ) conversion methods have shown the greatest potential to reduce soil Pb bioaccessibility, an in vitro bioaccessibility assay measurement of the proportion of Pb solubilized under gastric chemical conditions. Soils tested utilizing the recent PLJ method were found to have a Pb bioaccessibility of <1%, compared to original soils possessing bioaccessibility of >70%. However, this technique requires heat (95−100 °C) to promote mineral transformation. Jarosite-group minerals may incorporate multiple interlayer cations; therefore, we probed the potential for jarosite to remediate Pb via intercalation by reacting presynthesized potassium (K)-jarosite with aqueous Pb and/or Pb-contaminated soil at room temperature. Both K-jarosite and heated PLJ-treated samples were investigated by pairing bioaccessibility analyses with advanced bulk and spatially resolved X-ray absorption spectroscopy analyses. Samples treated with K-jarosite promoted Pb transformation to low-bioaccessibility (<10%) PLJ, with soil being converted to 100% PLJ using both heated and nonheated techniques. μ-X-ray fluorescence (μ-XRF) and μ-X-ray absorption near-edge structure (μ-XANES) showcase significant differences between elemental interactions for heated and nonheated PLJ-treated samples with anglesite impurities being found on the microscale. Although further development is necessary to accommodate for suitable field conditions, results indicate, for the first time, that K-jarosite may successfully convert soil Pb to PLJ without high-temperature conditions. The newfound utility of K-jarosite is expected to be key to future jarosite-based soil Pb remediation method development.