Lead Speciation, Bioaccessibility, and Sources for a Contaminated Subset of House Dust and Soils Collected from Similar United States Residences.

Residential lead (Pb) exposure is of critical concern to families globally as Pb promotes severe neurological effects in children, especially those less than 5 years old, and no blood lead level is deemed safe by the US Center for Disease Control. House dust and soils are commonly thought to be important sources of Pb exposure. Probing the relationship between house dust and soil Pb is critical to understanding residential exposure, as Pb bioavailability is highly influenced by Pb sources and/or species. We investigated paired house dust and soil collected from homes built before 1978 to determine Pb speciation, source, and bioaccessibility with the primary goal of assessing chemical factors driving Pb exposure in residential media. House dust was predominately found to contain (hydro)cerussite (i.e., Pb (hydroxy)carbonate) phases commonly used in Pb-based paint that, in-turn, promoted elevated bioaccessibility (>60%). Pb X-ray absorption spectroscopy, µ-XRF mapping, and Pb isotope ratio analysis for house dust and soils support house dust Pb as chemically unique compared to exterior soils, although paint Pb is expected to be a major source for both. Soil pedogenesis and increased protection from environmental conditions (e.g., weathering) in households is expected to greatly impact Pb phase differences between house dust and soils, subsequently dictating differences in Pb exposure.

United States house dust Pb concentrations are influenced by soil, paint, and house age: insights from a national survey.

BACKGROUND: Lead (Pb) in house dust contributes significantly to blood lead levels (BLLs) in children which may result in dire health consequences. Assessment of house dust Pb in the United States, relationships with Pb in soil and paint, and residential factors influencing Pb concentrations are essential to probing drivers of house dust Pb exposure. OBJECTIVE: Pb concentrations in vacuum-collected house dust are characterized across 346 homes participating in the American Health Homes Survey II (AHHS II), a US survey (2018-2019) evaluating residential Pb hazards. Connections between house dust Pb and soil Pb, paint Pb, and other residential factors are evaluated, and dust Pb concentration data are compared to paired loading data to understand Pb hazard standard implications. RESULTS: Mean and median vacuum dust Pb concentrations were 124 µg Pb g-1 and 34 µg Pb g-1, respectively. Vacuum-collected dust concentrations and dust wipe Pb loading rates were significantly correlated within homes (α < 0.001; r ≥ 0.4). At least one wipe sample exceeded current house dust Pb loading hazard standards (10 µg ft-2 or 100 µg Pb ft-2 for floors and windowsills, respectively) in 75 of 346 homes (22%). House dust Pb concentrations were correlated with soil Pb (r = 0.64) and Pb paint (r = 0.57). Soil Pb and paint Pb were also correlated (r = 0.6). IMPACT: The AHHS II provides a window into the current state of Pb in and around residences. We evaluated the relationship between house dust Pb concentrations and two common residential Pb sources: soil and Pb-based paint. Here, we identify relationships between Pb concentrations from vacuum-collected dust and paired Pb wipe loading data, enabling dust Pb concentrations to be evaluated in the context of hazard standards. This relationship, along with direct ties to Pb in soil and interior/exterior paint, provides a comprehensive assessment of dust Pb for US homes, crucial for formulating effective strategies to mitigate Pb exposure risks in households.

Potassium jarosite seeding of soils decreases lead and arsenic bioaccessibility: A path toward concomitant remediation.

Soils are common sources of metal(loid) contaminant exposure globally. Lead (Pb) and arsenic (As) are of paramount concern due to detrimental neurological and carcinogenic health effects, respectively. Pb and/or As contaminated soils require remediation, typically leading to excavation, a costly and environmentally damaging practice of removing soil to a central location (e.g., hazardous landfill) that may not be a viable option in low-income countries. Chemical remediation techniques may allow for in situ conversion of soil contaminants to phases that are not easily mobilized upon ingestion; however, effective chemical remediation options are limited. Here, we have successfully tested a soil remediation technology using potted soils that relies on converting soil Pb and As into jarosite-group minerals, such as plumbojarosite (PLJ) and beudantite, possessing exceptionally low bioaccessibility [i.e., solubility at gastric pH conditions (pH 1.5 to 3)]. Across all experiments conducted, all new treatment methods successfully promoted PLJ and/or beudantite conversion, resulting in a proportional decrease in Pb and As bioaccessibility. Increasing temperature resulted in increased conversion to jarosite-group minerals, but addition of potassium (K) jarosite was most critical to Pb and As bioaccessibility decreases. Our methods of K-jarosite treatment yielded <10% Pb and As bioaccessibility compared to unamended soil values of approximately 70% and 60%, respectively. The proposed treatment is a rare dual remediation option that effectively treats soil Pb and As such that potential exposure is considerably reduced. Research presented here lays the foundation for ongoing field application.

Successful Conversion of Pb-Contaminated Soils to Low-Bioaccessibility Plumbojarosite Using Potassium-Jarosite at Ambient Temperature.

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.

Interconnected soil iron and arsenic speciation effects on arsenic bioaccessibility and bioavailability: a scoping review.

Extensive research has examined arsenic (As) bioavailability in contaminated soils and is routinely assessed using in vitro bioaccessibility (IVBA) assays. Analysis of differences in bioaccessibility measurements across IVBA assays and phases is expected to provide valuable insights into geochemical mechanisms controlling soil As bioaccessibility and bioavailability. Soil iron (Fe) content and As speciation are expected to significantly influence IVBA gastric and intestinal phases due to fluctuations in precipitation-dissolution chemistry and sorption reactivity as pH and assay chemical complexity changes. The aim of this review was to examine these relationships by 1) conducting a meta-analysis (n = 47 soils) determining the influence of total Fe on As bioaccessibility measurements and 5 IVBA assays and 2) investigating the effect of As speciation on gastric/intestinal phase IVBA and in vitro-in vivo correlations. Our findings indicate that soil Fe content and As speciation heterogeneity are important in elucidating variability of bioaccessibility measurements across IVBA assays and gastrointestinal phases. Greater focus on coupled As speciation and Fe precipitation chemistry may (1) improve our understanding of soil geochemical factors and assay constituents that influence As in vitro-in vivo correlations and (2) resolve variability in the precision of oral relative bioavailability (RBA) estimated using IVBA assays for soils possessing heterogenous As speciation and Fe composition.

High Lead Bioavailability of Indoor Dust Contaminated with Paint Lead Species.

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 X-ray 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.