Legacy of anthropogenic lead in urban soils: Co-occurrence with metal(loids) and fallout radionuclides, isotopic fingerprinting, and in vitro bioaccessibility.

Anthropogenic lead (Pb) in soils poses risks to human health, particularly to the neuropsychological development of exposed children. Delineating the sources and potential bioavailability of soil Pb, as well as its relationship with other contaminants is critical in mitigating potential human exposure. Here, we present an integrative geochemical analysis of total elemental concentrations, radionuclides of 137Cs and 210Pb, Pb isotopic compositions, and in vitro bioaccessibility of Pb in surface soils sampled from different locations near Durham, North Carolina. Elevated Pb (>400 mg/kg) was commonly observed in soils from urban areas (i.e., near residential house foundation and along urban streets), which co-occurred with other potentially toxic metal(loids) such as Zn, Cd, and Sb. In contrast, soils from city parks and suburban areas had systematically lower concentrations of metal(loids) that were comparable to geological background. The activities of 137Cs and excess 210Pb, coupled with their correlations with Pb and co-occurring metal(loids) were used to indicate the persistence and remobilization of historical atmospherically deposited contaminants. Coupled with total Pb concentrations, the soil Pb isotopic compositions further indicated that house foundation soils had significant input of legacy lead-based paint (mean = 1.1895 and 2.0618 for 206Pb/207Pb and 208Pb/206Pb, respectively), whereas urban streetside soils exhibited a clear mixed origin, dominantly of legacy leaded gasoline (1.2034 and 2.0416) and atmospheric deposition (1.2004-1.2055 and 2.0484-2.0525). The in vitro bioaccessibility of Pb in contaminated urban soils furthermore revealed that more than half of Pb in the contaminated soils was potentially bioavailable, whose Pb isotope ratios were identical to that of bulk soils, demonstrating the utility of using Pb isotopes for tracking human exposure to anthropogenic Pb in soils and house dust. Overall, this study demonstrated a holistic assessment for comprehensively understanding anthropogenic Pb in urban soils, including its co-occurrence with other toxic contaminants, dominant sources, and potential bioavailability upon human exposure.

Characterization of adipogenic, PPARγ, and TRß activities in house dust extracts and their associations with organic contaminants.

In this study, we sought to expand our previous research on associations between bioactivities in dust and associated organic contaminants. Dust samples were collected from central NC homes (n = 188), solvent extracted, and split into two fractions, one for analysis using three different bioassays (nuclear receptor activation/inhibition and adipocyte development) and one for mass spectrometry (targeted measurement of 124 organic contaminants, including flame retardants, polychlorinated biphenyls, perfluoroalkyl substances, pesticides, phthalates, and polycyclic aromatic hydrocarbons). Approximately 80% of dust extracts exhibited significant adipogenic activity at concentrations that are comparable to estimated exposure for children and adults (e.g. ~20 µg/well dust) via either triglyceride accumulation (65%) and/or pre-adipocyte proliferation (50%). Approximately 76% of samples antagonized thyroid receptor beta (TRß), and 21% activated peroxisome proliferator activated receptor gamma (PPARγ). Triglyceride accumulation was significantly correlated with TRß antagonism. Sixty-five contaminants were detected in at least 75% of samples; of these, 26 were correlated with adipogenic activity and ten with TRß antagonism. Regression models were used to evaluate associations of individual contaminants with adipogenic and TRß bioactivities, and many individual contaminants were significantly associated. An exploratory g-computation model was used to evaluate the effect of mixtures. Contaminant mixtures were positively associated with triglyceride accumulation, and the magnitude of effect was larger than for any individually measured chemical. For each quartile increase in mixture exposure, triglyceride accumulation increased by 212% (RR = 3.12 and 95% confidence interval: 1.58, 6.17). These results suggest that complex mixtures of chemicals present in house dust may induce adipogenic activity in vitro at environmental concentrations and warrants further research.

Choice of vehicle affects pyraclostrobin toxicity in mice.

Pyraclostrobin is a strobilurin fungicide that inhibits mitochondrial complex III of fungal and mammalian cells. In toxicity studies that were used to estimate the safety factor, pyraclostrobin was added to animal feed or to aqueous vehicles. However, foods containing residues of pyraclostrobin and other strobilurin fungicides (azoxystrobin, trifloxystrobin, fluoxastrobin) are frequently prepared in vegetable oil prior to human consumption. The primary objective of this study was to determine if pyraclostrobin dissolved in an oil-based vehicle had adverse health outcomes in mice when compared to aqueous-based vehicles. We found that pyraclostrobin does not fully dissolve in aqueous methyl cellulose (MC) or carboxymethyl cellulose (CMC), two vehicles used in industry-sponsored toxicity studies, but does fully dissolve in corn oil. Moreover, C57BL/6 mice receiving pyraclostrobin in corn oil displayed adverse health outcomes, including loss of body weight, hypothermia and diarrhea at lower doses than when added to feed or to aqueous vehicles. Our data suggest that previous studies underestimated the true toxicity of pyraclostrobin in mammals. Additional toxicity tests using oil-based vehicles are recommended to verify current safety recommendations for strobilurin fungicides.