Matthew Lorber

Exposure of Americans to polybrominated diphenyl ethers

Polybrominated diphenyl ethers, PBDEs, are a class of brominated flame retardants that, like other persistent organic pollutants (POPs), have been found in humans, wildlife, and biota worldwide. Unlike other POPs, however, the key routes of human exposure are not thought to be food and fish, but rather are from their use in household consumer products, and to the high levels of PBDEs found in house dust. The exposure of Americans to PBDEs was systematically evaluated in this study. First, exposure media data on PBDE congeners were compiled. Then, an adult intake dose was derived using exposure factors in combination with these data. The exposure pathways evaluated included food and water ingestion, inhalation, and ingestion and dermal contact to house dust. These intakes were converted to a body burden using a simple pharmacokinetic (PK) model. The predicted body burdens were compared with representative profiles of PBDEs in blood and milk. The adult intake dose of total PBDEs was estimated to be 7.7 ng/kg body weight/day, and childrens estimated intakes were higher at 49.3 ng/kg/day for ages 1–5, 14.4 ng/kg/day for 6–11, and 9.1 ng/kg/day for 12–19. The much higher dose for the child age 1–5 was due to the doubling of dust ingestion from 50 to 100 mg/day. The predicted adult body burden of total PBDEs was 33.8 ng/kg lipid weight (lwt), compared to representative measurements in blood and milk at 64.0 and 93.7 ng/g lwt, respectively Most of this apparent underprediction in total concentration was due to an underprediction of the key congener, BDE 47. The value for BDE 47 half-life in the body was identified as the variable most likely in error in this exercise. Other congener predictions compared well with measurements, suggesting general validity with the approach. An important finding from this assessment is that the food intake estimate of about 1.3 ng/kg/day (of the 7.7 ng/kg/day total) cannot explain current US body burdens; exposures to PBDEs in house dust accounted for 82% of the overall estimated intakes.

The Pesticide Root Zone Model (PRZM): A procedure for evaluating pesticide leaching threats to groundwater

Abstract A continuous simulation model that considers interactions of pesticides in surface runoff (in water and on eroded sediment), advection in percolating water, molecular diffusion, dispersion, uptake by plants, sorption to soil, and biological and chemical degradation is described. The model was partially performance tested for aldicarb using data from field sites in New York, Florida, and Wisconsin. The model was successfully tested with observed data at the sites using selected values for 1st-order degradation rate constants and sorption coefficients. The model was successfully calibrated to the observed data at the New York site using selected values for 1st-order degradation rate constants and sorption coefficients. Calibrated parameter values were within the reported range of measured values, suggesting the model effectively simulates relevant processes affecting the pesticides movement. An example of model application for a hypothetical pesticide applied to wheat in Nebraska is provided.

Phthalate Concentrations and Dietary Exposure from Food Purchased in New York State

Background: Phthalates have been found in many personal care and industrial products, but have not previously been reported in food purchased in the United States. Phthalates are ubiquitous synthetic compounds and therefore difficult to measure in foods containing trace levels. Phthalates have been associated with endocrine disruption and developmental alteration. Objectives: Our goals were to report concentrations of phthalates in U.S. food for the first time, specifically, nine phthalates in 72 individual food samples purchased in Albany, New York, and to compare these findings with other countries and estimate dietary phthalate intake. Methods: A convenience sample of commonly consumed foods was purchased from New York supermarkets. Methods were developed to analyze these foods using gas chromatography–mass spectroscopy. Dietary intakes of phthalates were estimated as the product of the food consumption rate and concentration of phthalates in that food. Results: The range of detection frequency of individual phthalates varied from 6% for dicyclohexyl phthalate (DCHP) to 74% for di-2-ethylhexyl phthalate (DEHP). DEHP concentrations were the highest of the phthalates measured in all foods except beef [where di-n-octyl phthalate (DnOP) was the highest phthalate found], with pork having the highest estimated mean concentration of any food group (mean 300 ng/g; maximum, 1,158 ng/g). Estimated mean adult intakes ranged from 0.004 μg/kg/day for dimethyl phthalate (DMP) to 0.673 μg/kg/day for DEHP. Conclusions: Phthalates are widely present in U.S. foods. While estimated intakes for individual phthalates in this study were more than an order of magnitude lower than U.S. Environmental Protection Agency reference doses, cumulative exposure to phthalates is of concern and a more representative survey of U.S. foods is indicated.

A pharmacokinetic model for estimating exposure of Americans to dioxin-like compounds in the past, present, and future

Empirical evidence suggests that exposure of Americans to dioxin-like compounds was low during the early decades of the 20th century, then increased during the 1940s and 1950s, reaching a peak in the 1960s and 1970s, and progressively decreased to lower levels in the 1980s and 1990s. Such evidence includes dioxin analysis of carbon-dated sediment cores of lakes and rivers, preserved meat samples from different decades of the 20th century, and limited body burden measurements of dioxin-like compounds. Pinsky and Lorber (1998) summarized studies measuring 2,3,7,8-TCDD in blood and adipose tissue, and found a range of 10-20 pg/g (ppt) lipid during the 1970s, and 2-10 ppt lipid during the 1980s. This study reviews body burdens of dioxin toxic equivalents, TEQs, to find a range from approximately 50 to 80 ppt lipid during the 1970s, 30-50 ppt lipid during the 1980s, and 10-20 ppt lipid during the 1990s (TEQs comprised of the 17 dioxin and furan congeners only). Pinsky and Lorber (1998) investigated historical exposure trends for 2,3,7,8-TCDD by using a single-compartment, first-order pharmacokinetic model. The current study extends this prior effort by modeling dioxin TEQs instead of the single compound, 2,3,7,8-TCDD. TEQs are modeled as though they were a single compound, in contrast to an approach where the individual dioxin and furan congeners are modeled separately. It was found that body burdens of TEQs during the 1970s, 1980s and 1990s could be modeled by assuming a historical dose which began the century at low levels of approximately 0.5 pg TEQ/kg/day, rose during the middle decades of the 20th century to over 6 pg TEQ/kg/day, and declined to current levels of approximately 0.5 pg TEQ/kg/day. Trends in individual and population body burdens of TEQs are also investigated using this PK modeling framework. A key uncertainty of this effort - assuming that TEQs behave as though they were a single compound - is discussed and analyzed.

Screening Level Assessment of Risks Due to Dioxin Emissions from Burning Oil from the BP Deepwater Horizon Gulf of Mexico Spill

Between April 28 and July 19 of 2010, the U.S. Coast Guard conducted in situ oil burns as one approach used for the management of oil spilled after the explosion and subsequent sinking of the BP Deepwater Horizon platform in the Gulf of Mexico. The purpose of this paper is to describe a screening level assessment of the exposures and risks posed by the dioxin emissions from these fires. Using upper estimates for the oil burn emission factor, modeled air and fish concentrations, and conservative exposure assumptions, the potential cancer risk was estimated for three scenarios: inhalation exposure to workers, inhalation exposure to residents on the mainland, and fish ingestion exposures to residents. U.S. EPAs AERMOD model was used to estimate air concentrations in the immediate vicinity of the oil burns and NOAAs HYSPLIT model was used to estimate more distant air concentrations and deposition rates. The lifetime incremental cancer risks were estimated as 6 × 10(-8) for inhalation by workers, 6 × 10(-12) for inhalation by onshore residents, and 6 × 10(-8) for fish consumption by residents. For all scenarios, the risk estimates represent upper bounds and actual risks would be expected to be less.

An assessment of the exposure of Americans to perfluorooctane sulfonate: A comparison of estimated intake with values inferred from NHANES data

To better understand human exposure to perfluorinated compounds (PFCs), a model that assesses exposure to perfluorooctane sulfonate (PFOS) and its precursors from both an intake and a body burden perspective and combines the two with a simple pharmacokinetic (PK) model is demonstrated. Exposure pathways were modeled under “typical” and “contaminated” scenarios, for young children and adults. A range of intakes was also estimated from serum concentrations of PFOS reported in the National Health and Nutrition Examination Survey (NHANES) using a first-order 1-compartment PK model. Total PFOS intakes (medians summed over all pathways) were estimated as: 160 and 2200 ng/day for adults and 50 and 640 ng/day for children under typical and contaminated scenarios, respectively. Food ingestion appears to be the primary route of exposure in the general population. For children, the contribution from dust ingestion is nearly as great as from food ingestion. Pathway-specific contributions span several orders of magnitude and exhibit considerable overlap. PK modeling suggests central tendency PFOS intakes for adults range between 1.6 and 24.2 ng/kg-bw/day, and the forward-based intake estimates are within this range. The favorable comparison reported between the forward-modeled and the back-calculated range of intake predictions lends validity to the proposed framework.

Development and validation of an air-to-beef food chain model for dioxin-like compounds

A model for predicting concentrations of dioxin-like compounds in beef is developed and tested. The key premise of the model is that concentrations of these compounds in air are the source term, or starting point, for estimating beef concentrations. Vapor-phase concentrations transfer to vegetations that cattle consume, and particle-bound concentrations deposit onto soils and these vegetations as well. Congener-specific bioconcentration parameters, coupled with assumptions on cattle diet, transform soil and vegetative concentrations into beef fat concentrations. The premise of the validation exercise is that a profile of typical air concentrations of dioxin-like compounds in a United States rural environment is an appropriate observed independent data set, and that a representative profile of United States beef concentrations of dioxin-like compounds is an appropriate observed dependent result. These data were developed for the validation exercise. An observed concentration of dioxin toxic equivalents in whole beef of 0.48 ng/kg is compared with a predicted 0.36 ng/kg. Principal uncertainties in the approach are identified and discussed. A major finding of this exercise was that vapor phase transfers of dioxin-like compounds to vegetations that cattle consume dominate the estimation of final beef concentrations: over 80% of the modeled beef concentration was attributed to such transfers.

A simple pharmacokinetic model to characterize exposure of Americans to Di-2-ethylhexyl phthalate

A simple pharmacokinetic model to predict concentrations of metabolites of di-2-ethylhexyl phthalate, DEHP, in humans starting from intakes of DEHP was developed and applied. This model predicts serum and urine concentrations of five DEHP metabolites: MEHP, 5oxo-MEHP, 5OH-MEHP, 5cx-MEPP, and 2cx-MMHP. The model was calibrated using data from an individual who dosed himself with 48.5 mg DEHP, and then took blood and urine samples over a 44-h period. The calibrated model was then used in two applications: one on a second set of individuals whose exposure to DEHP was through PVC medical devices in a blood platelet donation procedure, and one on background exposures in the United States (US). Based on 2001/02 NHANES data, median US background urine concentrations of MEHP, 5OH-MEHP, and 5oxo-MEHP are 4.1, 20.1, and 14.0 μg/l, respectively. Creatine and urine volume-correction approaches were used to backcalculate an average daily dose of DEHP in the range of 0.6–2.2 μg/kg per day. A “background cohort” including 8 individuals and 57 complete days of urination were assumed to be exposed to1.5 μg/kg per day, spread out in equal doses of 0.3 μg/kg per day at 0900, 1200, 1500, 1800, and 2100 h. The average predicted urine concentrations were 4.6, 15.9, and 9.4 μg/l for MEHP, 5OH-MEHP, and 5oxo-MEHP. These are similar, but the two secondary metabolites are slightly lower than medians found in NHANES. This slight difference between the NHANES results and the background simulations could have been due to differences in metabolism between the individual who provided the calibration data (61-year-old Caucasian male) and the general US population. Another explanation evaluated was that urine concentrations further from the time of exposure may have larger disparities between MEHP and the two secondary metabolites as compared with concentrations measured closer to the time of exposure.

Population variability of phthalate metabolites and bisphenol A concentrations in spot urine samples versus 24- or 48-h collections.

Human exposure to phthalates and bisphenol A (BPA) can be assessed through urinary biomonitoring, but methods to infer daily intakes assume that spot sample concentrations are comparable to daily average concentrations. We evaluate this assumption using human biomonitoring data from Germany and the United States (US). The German data comprised three regional studies with spot samples and one with full-day samples analyzed for phthalate metabolites. The US data included: a study on DEHP metabolites and BPA involving eight persons supplying all urine voids (from which 24-h samples were constructed) for seven consecutive days; NHANES spot sample data on DEHP metabolites and BPA; and a regional study of children with 48-h samples analyzed for BPA. In the German data, measures of central tendency differed, but spot and 24-h samples showed generally comparable variance including 95th percentiles and maxima equidistant from central tendency measures. In contrast, the US adult data from the eight-person study showed similar central tendencies for phthalate metabolites and BPA, but generally greater variability for the spot samples, including higher 95th percentiles and maxima. When comparing childrens BPA concentrations in NHANES spot and 48-h samples, distributions showed similar central tendency and variability. Overall, spot urinary concentrations of DEHP metabolites and BPA have variability roughly comparable with corresponding 24-h average concentrations obtained from a comparable population, suggesting that spot samples can be used to characterize population distributions of intakes. However, the analysis also suggests that caution should be exercised when interpreting the high end of spot sample data sets.

Evaluation of background exposures of Americans to dioxin-like compounds in the 1990s and the 2000s

The US Environmental Protection Agencys 2004 Dioxin Reassessment included a characterization of background exposures to dioxin-like compounds, including an estimate of an average background intake dose and an average background body burden. These quantities were derived from data generated in the mid-1990s. Studies conducted in the 2000s were gathered in an attempt to update the estimates generated by the Reassessment. While these studies suggest declines in the average background dose and body burden, a precise quantification of this decline, much less a conclusion that a decline has indeed occurred, cannot be made because of the inconsistency of study design and data sources, and the treatment of non-detects in the generation of congener average concentrations. The average background intake of the Reassessment was 61.0 pg TEQ/day, and using more current data, the average background intake was 40.6 pg TEQ/day. The average body burden from the surveys in the mid-1990s was 22.9 pg TEQ/g lipid weight (pg/g lwt). More recent blood concentration data, from NHANES 2001/2, suggest an adult average at 21.7 pg/g TEQ lwt. These TEQ values include the 17 dioxin and furan congeners and 3 coplanar PCBs, and were generated substituting ND=(1/2)DL or ND=DL/sq rt (2). Results are provided for ND=0 and analyses conducted to evaluate the impacts of this substitution. A more detailed examination of beef and pork data from similarly designed national statistical surveys show that declines in pork are statistically significant while the beef concentrations appeared to have remained constant between the time periods.