Perfluoroalkyl Substances in U.S. market basket fish and shellfish.

Over the past two decades the class of per- and polyfluoroalkyl substances (PFAS) has emerged as a widespread contaminant in environmental media globally. As awareness and understanding of its prevalence, persistence, and potential health risks grows, so have concerns about human exposure. While drinking water has received substantial attention, dietary intakes have also been reported to contribute significantly to total exposure, with fish consumption in particular. Most studies of U.S. fish have targeted sport fish from areas of known or suspected contamination. This study was undertaken to improve data on PFAS levels in the U.S. commercial seafood supply. A total of 70 samples of finfish and shellfish were purchased at U.S. grocery stores and fish markets and analyzed for 26 PFAS compounds. The samples included a range of marine and freshwater species from four regions of the U.S. and seven countries with significant imports to the U.S. Up to ten PFAS were detected in 21 samples, with PFOS the predominant compound. There were no detections in the remaining 49 samples (detection limits of approximately 0.4-0.5 ppb). Total PFAS concentrations in most samples were single digit or sub-ppb levels. The exception was commercial finfish from the Great Lakes area, for which higher levels (up to 22 ppb) were observed in whitefish, walleye, and yellow perch fillet. Study findings suggest PFAS is present at low or non-detect levels in the U.S. commercial seafood supply and exposure is low for consumers of market basket fish and shellfish.

An investigation of homes with high concentrations of PCDDs, PCDFs, and/or dioxin-like PCBs in house dust.

As part of the University of Michigan Dioxin Exposure Study, the 29 congeners of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans, and dioxin-like polychlorinated biphenyls that have World Health Organization consensus toxic equivalency factors were measured in house dust from 764 homes using a population-based sampling design over selected regions in five Michigan counties. Twenty homes had a total toxic equivalency in house dust that was more than 2.5 standard deviations above the mean (i.e., defined to be outliers). This follow-up investigation describes the outlier house dust measurements and corresponding soil measurements and explores possible sources of these toxins in house dust. The congener distributions in the house dust outliers varied and were dominated (i.e., >50% of the total toxic equivalency) by either polychlorinated dibenzo-p-dioxins (n = 9), polychlorinated dibenzofurans (n = 1), or dioxin-like polychlorinated biphenyls (n = 9). Likely sources of contamination of house dust were identified in only three cases. In two cases, dust contamination appeared to be related to contaminated soil adjacent to the home; in one case, contamination was related to a source within the home (a carpet pad). In most cases, the source(s) of contamination of house dust could not be identified but appeared likely to be related to uncharacterized sources within the homes.

Case report: human exposure to dioxins from clay.

CONTEXT: For the general population, the dominant source of exposure to dioxin-like compounds is food. As part of the University of Michigan Dioxin Exposure Study (UMDES), we measured selected polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and dioxin-like polychlorinated biphenyls (PCBs) in serum of 946 subjects who were a representative sample of the general population in five Michigan counties. CASE PRESENTATION: The total toxic equivalency (TEQ; based on 2005 World Health Organization toxic equivalency factors) of serum from the index case was 211 ppt on a lipid-adjusted basis, which was the highest value observed in the UMDES study population. This subject had no apparent opportunity for exposure to dioxins, except that she had lived on property with soil contaminated with dioxins for almost 30 years, and had been a ceramics hobbyist for > 30 years. Soil from her property and clay that she used for ceramics were both contaminated with dioxins, but the congener patterns differed. DISCUSSION: The congener patterns in this subject's serum, soil, and ceramic clay suggest strongly that the dioxin contamination in clay and not soil was the dominant source of dioxin contamination in her serum. RELEVANCE TO PUBLIC HEALTH PRACTICE: It appears that ceramic clay, in particular the process of firing clay with unvented kilns, can be a significant nonfood and nonindustrial source of human exposure to dioxins among ceramics hobbyists. The extent of human exposure from ceramic clay is unclear, but it may be widespread. Further work is needed to more precisely characterize the routes of exposure.

Serum concentrations of polychlorinated dibenzo-p-dioxins among ceramicists.

Polychlorinated dibenzo-p-dioxins (PCDDs) occur naturally in ball clay at elevated concentrations. Thus, persons who habitually work with clay may be at risk for exposure to PCDDs. An earlier case report provided some evidence of elevated PCDD levels in serum for long-term hobby ceramicists; however, no previous study has measured serum dioxin concentrations among ceramicists. This study measured PCDD serum levels for 27 individuals involved in ceramics making. The average residual, defined as the average of the [log measured serum lipid concentration ­ log background serum lipid concentration], was calculated and then tested to determine whether it was significantly different from zero. The p-values for the average residuals indicated that the serum lipid concentrations for several PCDD congeners were elevated relative to background. The number of significant residuals increased dramatically if the background concentrations were adjusted to account for the fact that they were not contemporaneous with the measurements for the ceramicists. The ratio of the 1,2,3,6,7,8-HxCDD concentration to the 1,2,3,7,8,9-HxCDD concentration was greater than 1.0, unlike in ball clay, suggesting that although long-term working with ball clay elevates the PCDD levels in serum somewhat, it is not the predominant source of the PCDD body burden for ceramicists.

Evaluation of the release of dioxins and PCBs during kiln-firing of ball clay.

Ball clay is known to be naturally contaminated with high levels of polychlorinated di-benzo-p-dioxins (PCDDs). This study evaluated the potential for PCDD, polychlorinated dibenzofuran (PCDF) and polychlorinated biphenyl (PCB) release during the kiln firing of ball clay in an art studio. Toxic equivalence (TEQ) were calculated using World Health Organization (WHO) 2005 toxic equivalence factors (TEF) and congener concentrations. Ten bags of commercial ball clay were found to have an average TEQ of 1,370 nanograms/kilogram (ng kg(-1)) dry weight (dw), almost exclusively due to PCDDs (99.98% of TEQ). After firing, none of the 29 dioxin-like analytes was measured above the limits of detection (LOD) in the clay samples. Air samples were taken during firings using both low-flow and high-flow air samplers. Few low-flow air samples contained measurable levels of dioxin congeners above the LOD. The mean TEQ in the high volume air samples ranged from 0.07 pg m(-3) to 0.21 pg m(-3) when firing ball clay, and was 0.11 pg m(-3) when no clay was fired. These concentrations are within the range measured in typical residences and well-controlled industrial settings. The congener profiles in the high-flow air samples differed from the unfired clay; the air samples had a considerable contribution to the TEQ from PCDFs and PCBs. Given that the TEQs of all air samples were very low and the profiles differed from the unfired clay, it is likely that the PCDDs in dry ball clay were destroyed during kiln firing. These results suggest that inhalation of volatilized dioxins during kiln firing of dry ball clay is an unlikely source of exposure for vocational and art ceramicists.

Relationship between polychlorinated dibenzo-p-dioxin, polychlorinated dibenzofuran, and dioxin-like polychlorinated biphenyl concentrations in vegetation and soil on residential properties.

The University of Michigan Dioxin Exposure Study was undertaken to address concerns that the industrial discharge of dioxin-like compounds in the Midland, Michigan, USA area had resulted in the contamination of soil and vegetation in the Tittabawassee River floodplain and downwind of the incinerator in the City of Midland. The study included the analysis of 597 vegetation samples, predominantly grass and weeds, from residential properties selected through a multistage probabilistic sample design in the Midland area, and in Jackson and Calhoun Counties (Michigan), as a background comparison, for 29 polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and polychlorinated biphenyls (PCBs). The mean toxic equivalent (TEQ) of the house perimeter vegetation samples ranged from 4.2 to 377 pg/g. The ratio of TEQs (vegetation to soil) was about 0.3, with a maximum of 3.5. Based on a calculation of the similarity of the congener patterns between the soil and the vegetation, it appeared that the source of the contamination on the vegetation was the surrounding soil. This conclusion was supported by linear regression analysis, which showed that the largest contributor to the R(2) for the outcome variable of log(10) of the vegetation concentration was log(10) of the surrounding soil concentration. Models of vegetation contamination usually focus on atmospheric deposition and partitioning. The results obtained here suggest that the deposition of soil particles onto vegetation is a significant route of contamination for residential herbage. Thus, the inclusion of deposition of soil particles onto vegetation is critical to the accurate modeling of contamination residential herbage in communities impacted by historic industrial discharges of persistent organic compounds.

Residences with anomalous soil concentrations of dioxin-like compounds in two communities in Michigan, USA: a case study.

Most contamination of residential property soil with dioxin-like compounds occurs as a result of proximity to industrial activity that produces such compounds and, outside the industrially impacted zone, the soil concentrations are at background levels. However, as part of the University of Michigan Dioxin Exposure Study, residential properties in the lower peninsula of Michigan, USA, were identified that were located far enough from known sources of these compounds that the soil concentrations should have been at background levels and yet the toxic equivalent (TEQ) of some properties' soil was greater than 2.5 standard deviations above the mean background level. In the three cases presented here from Midland/Saginaw Counties, the anomalously high-TEQ values were primarily due to the presence of polychlorinated dibenzofurans. Based on interviews with the residents and a comparison of soil congener profiles, it was deduced that these values resulted from anthropogenic soil movement from historically contaminated areas. In the cases from Jackson/Calhoun Counties, the unusually high-TEQ values were primarily due to polychlorinated biphenyls. In the case profiled here, it appears that the soil became contaminated through sandblasting to remove paint from the swimming pool. This study identified two mechanisms for soil contamination outside zones of industrial impact; thus, an assumption of background levels of soil contamination outside industrial zones may not be valid.

The University of Michigan Dioxin Exposure Study: predictors of human serum dioxin concentrations in Midland and Saginaw, Michigan.

BACKGROUND: We conducted a population-based human exposure study in response to concerns among the population of Midland and Saginaw counties, Michigan, that discharges by the Dow Chemical Company of dioxin-like compounds into the nearby river and air had led to an increase in residents' body burdens of polychlorinated dibenzofurans (PCDDs), polychlorinated dibenzofurans (PCDFs), and dioxin-like polychlorinated biphenyls (PCBs), here collectively referred to as "dioxins." OBJECTIVES: We sought to identify factors that explained variation in serum dioxin concentrations among the residents of Midland and Saginaw counties. Exposures to dioxins in soil, river sediments, household dust, historic emissions, and contaminated fish and game were of primary interest. METHODS: We studied 946 people in four populations in the contaminated area and in a referent population, by interview and by collection of serum, household dust, and residential soil. Linear regression was used to identify factors associated with serum dioxins. RESULTS: Demographic factors explained a large proportion of variation in serum dioxin concentrations. Historic exposures before 1980, including living in the Midland/Saginaw area, hunting and fishing in the contaminated areas, and working at Dow, contributed to serum dioxin levels. Exposures since 1980 in Midland and Saginaw counties contributed little to serum dioxins. CONCLUSIONS: This study provides valuable insights into the relationships between serum dioxins and environmental factors, age, sex, body mass index, smoking, and breast-feeding. These factors together explain a substantial proportion of the variation in serum dioxin concentrations in the general population. Historic exposures to environmental contamination appeared to be of greater importance than recent exposures for dioxins.