Perfluoroalkyl substances and food allergies in adolescents

Perfluoroalkyl and polyfluoroalkyl substances (PFASs) are a class of organic compounds that are persistent in the environment due to their stable carbon-fluorine backbone, which is not susceptible to degradation. Research suggests these chemicals may exert an immunotoxic effect. The aim of this study is to investigate the associations between four PFASs – perfluorooctane sulfonic acid (PFOS), perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), and perfluorohexane sulfonic acid (PFHxS) – with food sensitization and food allergies in adolescent participants (ages 12–19 years) in the National Health and Nutrition Examination Survey (NHANES) 2005–2006 and 2007–2010, respectively. We performed multivariate logistic regression to analyze the association between individual PFASs with food sensitization (defined as having at least 1 food-specific IgE level ≥ 0.35 kU/L) in NHANES 2005–2006 and food allergies (self-reported) in NHANES 2007–2010. Serum PFOA, PFOS, and PFHxS were statistically significantly associated with higher odds to have self-reported food allergies in NHANES 2007–2010. When using IgE levels as a marker of food sensitization, we found that serum PFNA was inversely associated with food sensitization (NHANES 2005–2006). In conclusion, we found that serum levels of PFASs were associated with higher odds to have self-reported food allergies. Conversely, adolescents with higher serum PFNA were less likely to be sensitized to food allergens. These results, along with previous studies, warrant further investigation, such as well-designed longitudinal studies.     

Changes in epidemiologic associations with different exposure metrics: A case study of phthalate exposure associations with body mass index and waist circumference

The use of human biomonitoring data to characterize exposure to environmental contaminants in epidemiology studies has expanded greatly in recent years. Substantial variability in effect measures may arise when using different exposure metrics for a given contaminant, and it is often not clear which metric is the best surrogate for the ‘causal’ or ‘true’ exposure. Here we evaluated variability and potential bias in epidemiologic associations resulting from the use of different phthalate exposure metrics in the 2009–2010 National Health and Nutrition Examination Survey (NHANES). We examined associations between urinary phthalate metabolites and the outcomes of body mass index (BMI) and waist circumference (WC). We examined each of the following NHANES-derived exposure metrics for metabolites of individual phthalates: molar excretion rate (nmol/min), molar amount (nmol), molar concentration (nmol/mL, with and without additional model adjustment for creatinine), creatinine corrected molar concentration (nmol/g creatinine), and reconstructed daily phthalate intake (nmol/kg/day). In order to investigate potential biasing effect of each metric, we first assumed that daily intake of the parent phthalate is the causal exposure. We then constructed a simulated population based on the 2009–2010 NHANES, and randomly assigned each individual a di-2-ethylhexyl phthalate (DEHP) intake dose based on a published distribution, but independent of any other factor. Accordingly, all associations between these randomly assigned intake doses and individuals' BMI and WC should be null. Next, demographic data in the NHANES were incorporated into a pharmacokinetic model to predict urinary molar excretions of five DEHP metabolites based on the randomly assigned DEHP intake. The predicted molar excretions were then used to calculate the same exposure metrics listed above. Three exposure metrics (randomly generated intake, excretion rate, urine concentration) showed no significant associations with BMI, which supports the null hypothesis stated above. In contrast, metrics adjusted for creatinine showed a significant negative correlation, and reconstructed daily intake showed a significant positive correlation, indicating the introduction of bias away from the true (i.e., null) association. Interestingly, trends in the simulation analysis were similar to those seen in the observed NHANES data. Our findings show that, at least in this example case, the choice of exposure metric can introduce significant bias of varying magnitude and direction into the calculation of epidemiologic associations.     

Temporal trends of perfluorooctanesulfonate isomer and enantiomer patterns in archived Swedish and American serum samples

Human perfluorooctanesulfonate (PFOS) body burdens are attributable to both direct PFOS and indirect PFOS precursor (PreFOS) exposure. The relative importance of these two pathways has been estimated, but the relative temporal trajectory of exposure to PFOS and PreFOS has not been examined. Here, two hypothesized biomarkers of PreFOS exposure, PFOS isomer profiles (quantified as percent branched PFOS, %br-PFOS) and chiral 1m-PFOS enantiomer fractions (1m-PFOS EF) were analyzed in archived human serum samples of individual American adults (1974–2010) and pooled samples of Swedish primiparous women (1996–2010). After correcting for potential confounders, significant correlations between %br-PFOS and 1m-PFOS EFs were observed in American samples and in Swedish samples for the 1996–2000 period, supporting the hypothesis that both %br-PFOS and 1m-PFOS EF are biomarkers of PreFOS exposure. Significant trends of increasing %br-PFOS, from 2000 to 2010, and increasingly non-racemic 1m-PFOS EFs, from 1996 to 2000, were detected in Swedish samples. No statistically significant trend for %br-PFOS or 1m-PFOS EF was observed in American samples, but American males had significantly higher %br-PFOS and significantly lower 1m-PFOS EF (i.e. more non-racemic) than females, and a similar significant difference was shown in the older age group, relative to the younger age group. These temporal trends in %br-PFOS and 1m-PFOS EF are not easily explained and the results highlight uncertainties about how humans are exposed to PFOS.     

Concentrations of polybrominated diphenyl ethers (PBDEs) in matched samples of human milk,dust and indoor air

Polybrominated diphenyl ethers (PBDEs) are lipophilic, persistent pollutants found worldwide in environmental and human samples. Exposure pathways for PBDEs remain unclear but may include food, air and dust. The aim of this study was to conduct an integrated assessment of PBDE exposure and human body burden using 10 matched samples of human milk, indoor air and dust collected in 2007–2008 in Brisbane, Australia. In addition, temporal analysis was investigated comparing the results of the current study with PBDE concentrations in human milk collected in 2002–2003 from the same region.PBDEs were detected in all matrices and the median concentrations of BDEs -47 and -209 in human milk, air and dust were: 4.2 and 0.3 ng/g lipid; 25 and 7.8 pg/m³; and 56 and 291 ng/g dust, respectively. Significant correlations were observed between the concentrations of BDE-99 in air and human milk (r = 0.661, p = 0.038) and BDE-153 in dust and BDE-183 in human milk (r = 0.697, p = 0.025). These correlations do not suggest causal relationships — there is no hypothesis that can be offered to explain why BDE-153 in dust and BDE-183 in milk are correlated. The fact that so few correlations were found in the data could be a function of the small sample size, or because additional factors, such as sources of exposure not considered or measured in the study, might be important in explaining exposure to PBDEs. There was a slight decrease in PBDE concentrations from 2002–2003 to 2007–2008 but this may be due to sampling and analytical differences. Overall, average PBDE concentrations from these individual samples were similar to results from pooled human milk collected in Brisbane in 2002–2003 indicating that pooling may be an efficient, cost-effective strategy of assessing PBDE concentrations on a population basis.The results of this study were used to estimate an infant's daily PBDE intake via inhalation, dust ingestion and human milk consumption. Differences in PBDE intake of individual congeners from the different matrices were observed. Specifically, as the level of bromination increased, the contribution of PBDE intake decreased via human milk and increased via dust. As the impacts of the ban of the lower brominated (penta- and octa-BDE) products become evident, an increased use of the higher brominated deca-BDE product may result in dust making a greater contribution to infant exposure than it does currently.To better understand human body burden, further research is required into the sources and exposure pathways of PBDEs and metabolic differences influencing an individual's response to exposure. In addition, temporal trend analysis is necessary with continued monitoring of PBDEs in the human population as well as in the suggested exposure matrices of food, dust and air.     

Is there a correlation between the number of mutagens and the number of nonmutagens in an environmental sample?

We have adapted a procedure which was developed for studying the correlations in the distribution of genetic factors, such as sex ratios in siblings, to obtain estimates of the correlation between the number of mutagens and the number of nonmutagens in a sample. Positive correlations with correlation coefficients in excess of 0.8 were obtained. The high correlation suggests that it is possible to estimate the number of mutagens in samples with N > 100 compounds as (0.064 ± 0.01) N.     

A temporal trend study (1972-2008) of perfluorooctanesulfonate, perfluorohexanesulfonate, and perfluorooctanoate in pooled human milk samples from Stockholm, Sweden

The widespread presence of perfluorooctanesulfonate (PFOS), perfluorooctanoate (PFOA), and perfluorohexanesulfonate (PFHxS) in human general populations and their slow elimination profiles have led to renewed interest in understanding the potential human neonatal exposures of perfluoroalkyls (PFAs) from consumption of human milk. The objective of this study was to evaluate the concentrations of PFOS, PFHxS, and PFOA in pooled human milk samples obtained in Sweden between 1972 and 2008 (a period representing the most significant period of PFA production) and to see whether the time trend of these analytes parallels that indicated in human serum. Chemical analysis of PFOS, PFHxS, and PFOA was performed on pooled Swedish human milk samples from 1972 to 2008 after methodological refinements. The 20 samples which formed the 2007 pool were also analyzed individually to evaluate sample variations. Analyses were performed by HPLC-MS/MS. Due to the complexities of the human milk matrix and the requirement to accurately quantitate low pg/mL concentrations, meticulous attention must be paid to background contamination if accurate results are to be obtained. PFOS was the predominant analyte present in the pools and all three analytes showed statistically significant increasing trends from 1972 to 2000, with concentrations reaching a plateau in the 1990s. PFOA and PFOS showed statistically significant decreasing trends during 2001-2008. At the end of the study, in 2008, the measured concentrations of PFOS, PFHxS, and PFOA in pooled human milk were 75 pg/mL, 14 pg/mL, and 74 pg/mL, respectively. The temporal concentration trends of PFOS, PFHxS, and PFOA observed in human milk are parallel to those reported in the general population serum concentrations.     

EPA's SHEDS-multimedia model: Children's cumulative pyrethroid exposure estimates and evaluation against NHANES biomarker data

The U.S. EPA's SHEDS-Multimedia model was applied to enhance the understanding of children's exposures and doses to multiple pyrethroid pesticides, including major contributing chemicals and pathways. This paper presents combined dietary and residential exposure estimates and cumulative doses for seven commonly used pyrethroids, and comparisons of model evaluation results with NHANES biomarker data for 3-PBA and DCCA metabolites. Model input distributions were fit to publicly available pesticide usage survey data, NHANES, and other studies, then SHEDS-Multimedia was applied to estimate total pyrethroid exposures and doses for 3–5 year olds for one year variability simulations. For dose estimations we used a pharmacokinetic model and two approaches for simulating dermal absorption. SHEDS-Multimedia predictions compared well to NHANES biomarker data: ratios of 3-PBA observed data to SHEDS-Multimedia modeled results were 0.88, 0.51, 0.54 and 1.02 for mean, median, 95th, and 99th percentiles, respectively; for DCCA, the ratios were 0.82, 0.53, 0.56, and 0.94. Modeled time-averaged cumulative absorbed dose of the seven pyrethroids was 3.1 nmol/day (versus 8.4 nmol/day for adults) in the general population (residential pyrethroid use and non-use homes) and 6.7 nmol/day (versus 10.5 nmol/day for adults) in the simulated residential pyrethroid use population. For the general population, contributions to modeled cumulative dose by chemical were permethrin (60%), cypermethrin (22%), and cyfluthrin (16%); for residential use homes, contributions were cypermethrin (49%), permethrin (29%), and cyfluthrin (17%). The primary exposure route for 3–5 year olds in the simulated residential use population was non-dietary ingestion exposure; whereas for the simulated general population, dietary exposure was the primary exposure route. Below the 95th percentile, the major exposure pathway was dietary for the general population; non-dietary ingestion was the major pathway starting below the 70th percentile for the residential use population. The new dermal absorption methodology considering surface loading had some impact, but did not change the order of key pathways.     

Estrogen-, androgen- and aryl hydrocarbon receptor mediated activities in passive and composite samples from municipal waste and surface waters

Passive and composite sampling in combination with in vitro bioassays and identification and quantification of individual chemicals were applied to characterize pollution by compounds with several specific modes of action in urban area in the basin of two rivers, with 400,000 inhabitants and a variety of industrial activities. Two types of passive samplers, semipermeable membrane devices (SPMD) for hydrophobic contaminants and polar organic chemical integrative samplers (POCIS) for polar compounds such as pesticides and pharmaceuticals, were used to sample wastewater treatment plant (WWTP) influent and effluent as well as rivers upstream and downstream of the urban complex and the WWTP. Compounds with endocrine disruptive potency were detected in river water and WWTP influent and effluent. Year-round, monthly assessment of waste waters by bioassays documented estrogenic, androgenic and dioxin-like potency as well as cytotoxicity in influent waters of the WWTP and allowed characterization of seasonal variability of these biological potentials in waste waters. The WWTP effectively removed cytotoxic compounds, xenoestrogens and xenoandrogens. There was significant variability in treatment efficiency of dioxin-like potency. The study indicates that the WWTP, despite its up-to-date technology, can contribute endocrine disrupting compounds to the river. Riverine samples exhibited dioxin-like, antiestrogenic and antiandrogenic potencies. The study design enabled characterization of effects of the urban complex and the WWTP on the river. Concentrations of PAHs and contaminants and specific biological potencies sampled by POCIS decreased as a function of distance from the city.     

Morphology,spatial distribution,and concentration of flame retardants in consumer products and environmental dusts using scanning electron microscopy and Raman micro-spectroscopy

We characterized flame retardant (FR) morphologies and spatial distributions in 7 consumer products and 7 environmental dusts to determine their implications for transfer mechanisms, human exposure, and the reproducibility of gas chromatography–mass spectrometry (GC–MS) dust measurements. We characterized individual particles using scanning electron microscopy/energy dispersive x-ray spectroscopy (SEM/EDS) and Raman micro-spectroscopy (RMS). Samples were screened for the presence of 3 FR constituents (bromine, phosphorous, non-salt chlorine) and 2 metal synergists (antimony and bismuth). Subsequent analyses of select samples by RMS enabled molecular identification of the FR compounds and matrix materials. The consumer products and dust samples possessed FR elemental weight percents of up to 36% and 31%, respectively. We identified 24 FR-containing particles in the dust samples and classified them into 9 types based on morphology and composition. We observed a broad range of morphologies for these FR-containing particles, suggesting FR transfer to dust via multiple mechanisms. We developed an equation to describe the heterogeneity of FR-containing particles in environmental dust samples. The number of individual FR-containing particles expected in a 1-mg dust sample with a FR concentration of 100 ppm ranged from < 1 to > 1000 particles. The presence of rare, high-concentration bromine particles was correlated with decabromodiphenyl ether concentrations obtained via GC–MS. When FRs are distributed heterogeneously in highly concentrated dust particles, human exposure to FRs may be characterized by high transient exposures interspersed by periods of low exposure, and GC–MS FR concentrations may exhibit large variability in replicate subsamples. Current limitations of this SEM/EDS technique include potential false negatives for volatile and chlorinated FRs and greater quantitation uncertainty for brominated FR in aluminum-rich matrices.     

Prenatal exposure to PCB-153, p,p′-DDE and birth outcomes in 9000 mother–child pairs: Exposure–response relationship and effect modifiers

Low-level exposure to polychlorinated biphenyl-153 (PCB-153) and dichlorodiphenyldichloroethylene (p-p′-DDE) can impair fetal growth; however, the exposure–response relationship and effect modifiers of such association are not well established. This study is an extension of an earlier European meta-analysis. Our aim was to explore exposure–response relationship between PCB-153 and p-p′-DDE and birth outcomes; to evaluate whether any no exposure–effect level and susceptible subgroups exist; and to assess the role of maternal gestational weight gain (GWG). We used a pooled dataset of 9377 mother–child pairs enrolled in 14 study populations from 11 European birth cohorts. General additive models were used to evaluate the shape of the relationships between organochlorine compounds and birth outcomes. We observed an inverse linear exposure–response relationship between prenatal exposure to PCB-153 and birth weight [decline of 194 g (95% CI − 314, − 74) per 1 μg/L increase in PCB-153]. We showed effects on birth weight over the entire exposure range, including at low levels. This reduction seems to be stronger among children of mothers who were non-Caucasian or had smoked during pregnancy. The most susceptible subgroup was girls whose mothers smoked during pregnancy. After adjusting for absolute GWG or estimated fat mass, a reduction in birth weight was still observed. This study suggests that the association between low-level exposure to PCB-153 and birth weight exists and follows an inverse linear exposure–response relationship with effects even at low levels, and that maternal smoking and ethnicity modify this association.     

Chronic risk assessment of exposure to volatile organic compounds in the atmosphere near the largest Mediterranean industrial site

This study focuses on characterising the risk of exposure to volatile organic compounds (VOCs) by means of inhalation in people living in the vicinity of the largest chemical production site in the Mediterranean area. Eighty-six VOCs were initially selected for this study based on their adverse environmental and health effects. The monitoring campaign was conducted for 276 days in three different locations around the chemical site. The analytical method used for the characterisation was based on European standard method EN-14662-2, which consists of the active sampling of air for 24 h in charcoal tubes, followed by extraction with carbon disulphide and GC-MS analysis. Forty-four VOCs with toxicological data available concerning their carcinogenic and non-carcinogenic health effects were quantified during the monitoring campaign. None of the quantified VOCs showed average concentrations exceeding their chronic reference concentrations and, therefore, no non-carcinogenic health effects are expected as a result of this exposure. However, the global average cancer risk due to VOC exposure in the area (3.3 × 10^− 4) was found to be above the values recommended by the WHO and USEPA.The influence of the analytical method was also evaluated by comparing cancer risk estimates using a thermal desorption (TD) method based on method EN-14662-1. The results of the 24-h samples for the solvent extraction method were compared with the average of 12 daily samples of 2-h for the TD method for 24 sampling days. Although the global estimated lifetime cancer risk was statistically comparable for both methods, some differences were found in individual VOC risks.To our knowledge, this is the first study that estimates the carcinogenic and non-carcinogenic risks posed by the inhalation of VOCs in people living near a chemical site of this size, and compares the estimated cancer risk obtained using two different standard analytical methods.     

Human biomonitoring of multiple mycotoxins in the Belgian population: Results of the BIOMYCO study

Mycotoxins are important food contaminants responsible for health effects such as cancer, nephrotoxicity, hepatotoxicity or immunosuppression. The assessment of mycotoxin exposure is often based on calculations combining mycotoxin occurrence data in food with population data on food consumption. Because of limitations inherent to that approach, the direct measurement of biomarkers of exposure in biological fluids has been proposed as a suitable alternative to perform an accurate mycotoxin exposure assessment at individual level. For this reason, the BIOMYCO study was designed to assess mycotoxin exposure in Belgian adults and children using urinary biomarkers of exposure. Morning urine was gathered in a representative part of the Belgian population according to a standardised study protocol, whereby 155 children (3–12 years old) and 239 adults (19–65 years old) were selected based on random cluster sampling. These urine samples were analysed for the presence of 33 potential biomarkers with focus on aflatoxins, citrinin (CIT), fumonisins, trichothecenes, ochratoxin A (OTA), zearalenone and their metabolites using two validated LC–MS/MS methods.Nine out of the 33 analysed mycotoxins were detected whereby deoxynivalenol (DON), OTA, CIT and their metabolites were the most frequently detected. Deoxynivalenol-15-glucuronide was the main urinary DON biomarker and was found in all urine samples in the ng/mL range. Furthermore deoxynivalenol-3-glucuronide was quantified in 91% of the urine samples collected from children and in 77% of the samples collected from adults. Deoxynivalenol was detected in 70% and 37% of the samples of children and adults respectively. For the first time deepoxy-deoxynivalenol-glucuronide was detected in children's urine (17%). In the samples collected by adults, the prevalence was 22%. Whereas all these mycotoxins contaminated the urine samples in the ng/mL range, CIT and OTA were present in much lower concentrations (pg/mL). OTA contaminated 51% and 35% of the samples collected by children and adults respectively. CIT and its metabolite were present in 72% and 6% of children's urine, whereas they contaminated 59% and 12% of adult's urine. Finally, α-zearalenol and β-zearalenol-14-glucuronide were found in respectively one and two samples from adults. The exposure to DON, OTA and CIT was compared between subgroups and urinary mycotoxin concentrations differed significantly among age and gender. Based on the urinary levels, the daily intake of DON and OTA was estimated and evaluated whereby, depending on the used method, 16–69% of the population possibly exceeded the tolerable daily intake for DON and 1% for OTA.The BIOMYCO study is the first study whereby a multi-toxin approach was applied for mycotoxin exposure assessment in adults and children on a large-scale. Moreover, it is the first study that described the exposure to an elaborated set of mycotoxins in the Belgian population. Biomarker analysis showed a clear exposure of a broad segment of the Belgian population to DON, OTA and CIT. The risk assessment based on these data indicates a potential concern for a number of individuals whereby young children need special attention because of the relatively higher food intake per kg body weight.     

Population Density and Fertility in Farm Households: A Study of the Millennium Development Authority Zones in Ghana

Agriculture is mainly a rural preoccupation, and about three quarters of the population growth in developing countries emanate from agricultural households. Some demographers posit that the agricultural system affects birth rates; in addition, population pressures might put stress on agricultural land in farming communities. This paper focuses on the population to land ratio in the Millennium Development Authority (MiDA) Enumeration Areas (EAs) in Ghana and tackles the important question: Do households adjust to an increasing population/land ratio by having fewer children? The authors explore this theme in the context of rural population density and fertility in the three MiDA zones, drawing on data collected in 23 EAs in Ghana in 2008. The results suggest that fertility in the MiDA zones can be affected by density if nothing is done to regulate population density. The regression estimates for the pooled data show that all the coefficients are negative and statistically significant at the 0.05 level or better. Thus, children ever born is inversely correlated with density, agricultural production, female literacy and the trend variable (year). The estimates from the cross-sectional data as well as the spatial coefficient were consistent with those of the pooled data. The results under various model specifications are stable. We find from the Cox model that areas with higher education levels and a lower share of individuals working in agriculture, both correlated with land use. Agricultural production has at most a modest independent effect on fertility. Our findings suggest that population density has a reasonable inhibiting effect on fertility in the MiDA Zones.     

Biota-sediment accumulation factors for Dechlorane Plus in bottom fish from an electronic waste recycling site,South China

Biota-sediment accumulation factors (BSAFs) for Dechlorane Plus (DP), a highly chlorinated flame retardant, were determined in three bottom fish species, i.e., crucian carp, mud carp, and northern snakehead from an electronic waste recycling site in South China. The average BSAFs are 0.007, 0.01, and 0.06 for syn-DP, and 0.003, 0.025, and 0.001 for anti-DP in crucian carp, mud carp, and northern snakehead, respectively, suggesting low bioaccumulation potential of DP isomers in these fish. However, the bioaccumulation factors (BAFs) determined previously in the same sample set indicated that both DP isomers were highly bioaccumulative (BAFs > 5000) in most of the samples. This implies that BSAF values may be inherently inconsistent affecting their reliability as a bioaccumulation indicator. The BSAFs for DP isomers are two orders of magnitude lower than those (average of 0.43–2.28) for extremely hydrophobic polychlorinated biphenyls (CBs 199, 203, 207 and 208), but are comparable to those (average of 0.0001–0.009) for decabromodiphenyl ether (BDE 209) determined in the same sample set. Despite of the different chemical structures of the three compound classes, significantly negative correlations between logarithm of octanol–water partition coefficients (log K_OWs) and BSAFs of these chemicals were found, indicating that hydrophobicity is one of the key factors influencing the bioaccumulation of these compounds.     

Biomarkers of pesticide exposure and diabetes in the 1999–2004 National Health and Nutrition Examination Survey

The associations of 8 pesticides and pesticide metabolites with total diabetes (diagnosed and undiagnosed) and pre-diabetes (glycohemoglobin 5.7–6.4%) were evaluated using the National Health and Nutrition Examination Survey (NHANES), 1999–2004. Six of the pesticides were found to be associated with total diabetes in separate adjusted logistic regressions. These pesticides and pesticide metabolites were beta-hexachlorocyclohexane, p,p′-DDE, p,p′-DDT, oxychlordane, trans-nonachlor, and heptachlor epoxide. When the number of compounds elevated was tested, 4 or more, of the 6, elevated had an odds ratio of 4.99 (95% CI 1.97–12.61) compared to none elevated. When the 6 compounds were tested together in a single combined adjusted logistic regression only oxychlordane, a metabolite of chlordane, and heptachlor epoxide, a metabolite of heptachlor, were significantly associated with total diabetes. In the combined adjusted logistic regression, oxychlordane ≥ 14.5 ng/g lipid adjusted had an odds ratios of 1.90 (95% CI 1.09–3.32) compared to oxychlordane < 14.5 ng/g lipid adjusted, and heptachlor epoxide ≥ 14.6 ng/g lipid adjusted had an odds ratio of 1.70 (95% CI 1.16–2.49) compared to heptachlor epoxide < 14.6 ng/g lipid adjusted. Heptachlor epoxide and p,p′-DDT were significantly associated with pre-diabetes in separate adjusted logistic regressions. When these 2 compounds were tested together only heptachlor epoxide remained significantly associated with pre-diabetes. The evidence supporting the relationship between pesticides and pesticide metabolites, with diabetes, was strongest for heptachlor epoxide and oxychlordane, intermediate for p,p′-DDT, and least for beta-hexachlorocyclohexane, p,p′-DDE, and trans-nonachlor. Mirex and dieldrin were not associated with total diabetes or pre-diabetes.     

Characterisation of NOM by adsorption parameters and effective diffusivities

Adsorption equilibria were studied with RO isolates for both activated carbon and activated alumina. Maximum carbon loadings on the order of 65 mg/g DOC were obtained, while the maximum loadings of activated alumina were about 30 mg/g DOC. In the latter case the slope of the isotherms was generally steeper, indicating weaker adsorbabilities of some of the NOM compounds on the metal oxide adsorbent. Since NOM must be regarded as a multi-component system with respect to adsorption, the data were evaluated by the adsorption analysis procedure. The results were used for a theoretical comparison of NOM adsorption based on the same initial concentration of all samples. The method of colloidal titration was applied to the RO isolates in the range pH = 3–8. Poly-DADMAC was used as a cationic polymer, and a streaming current instrument was used for end point detection. The results which are termed anionic colloidal charge (ACC) values increase with increasing pH for pH = 3–6 while they are about constant for pH = 6–8. At the samples' original pH, the specific ACC values found range from 5.2 to 7.6 meq/g DOC. Mass transfer coefficients for NOM adsorption on granular activated carbon were determined for both RO and EVAP isolates, respectively. The data were used to derive effective diffusivities for each sample. The results differ by a factor of about 2 with the Maridalsvann sample having the highest and the Humex sample having the lowest diffusivity. Furthermore, the results for the EVAP isolates are in 8 of 9 cases higher than for the RO samples. Based on a comparison with known macromolecules, average molecular weight values were estimated to be on the order of 700–4800 Dalton.     

An approach to assessing the probability of unsatisfactory radon in air-conditioned offices of Hong Kong

In order to maintain an acceptable Indoor Air Quality (IAQ), policies, strategies and guidelines have been developed worldwide and exposure concentrations of the indoor radon have been specified. Mapping indoor radon levels for a region could be done with intensive measurements on a large number of samples. To obtain the most accurate estimate of the levels with the uncertainties specified, a statistical model has been developed in this study to predict the fractions of samples in a region having an average radon level above the action levels of 150Bqm(-3) and 200Bqm(-3). The model was based on a transformation of the variation from a small sample set of data to a population geometric distribution via an estimator, known as the 'sample correction factor'. Using a dataset from a cross-sectional measurement of indoor radon levels in 216 Hong Kong offices, where the mean was 37.2Bqm(-3) and the 68% range was from 17.3Bqm(-3) to 80.3Bqm(-3), the 'sample correction factor' was evaluated and tested by the Monte-Carlo simulations. The model estimates of the fractions above the indoor radon action levels 150Bqm(-3) and 200Bqm(-3) (1.2-7.7% and 0.4-4.1% for a sample size of 20, 2.8-5.1% and 0.8-2.4% for a sample size of 60) were demonstrated to be consistent with those determined from the dataset (3.5% and 1.4%). With the 'sample correction factor' thus quantified, it will be possible to provide the required data for the policymakers making appropriate decisions on resources and manpower management.     

Monitoring exposure to polycyclic aromatic hydrocarbons in an Australian population using pooled urine samples

Integrated exposure to polycyclic aromatic hydrocarbons (PAHs) can be assessed through monitoring of urinary mono-hydroxylated PAHs (OH-PAHs). The aim of this study was to provide the first assessment of exposure to PAHs in a large sample of the population in Queensland, Australia including exposure to infant (0–4 years). De-identified urine specimens, obtained from a pathology laboratory, were stratified by age and sex, and pooled (n = 24 pools of 100) and OH-PAHs were measured by gas chromatography–isotope dilution–tandem mass spectrometry. Geometric mean (GM) concentrations ranged from 30 ng/L (4-hydroxyphenanthrene) to 9221 ng/L (1-naphthol). GM of 1-hydroxypyrene, the most commonly used PAH exposure biomarker, was 142 ng/L. The concentrations of OH-PAHs found in this study are consistent with those in developed countries and lower than those in developing countries. We observed no association between sex and OH-PAH concentrations. However, we observed lower urinary concentrations of all OH-PAHs in samples from infants (0–4 years), children (5–14 years) and the elderly (> 60 year old) compared with samples from other age groups (15–29, 30–44 and 45–59 years) which may be attributed to age-dependent behaviour-specific exposure sources.     

The use of ambient air quality modeling to estimate individual and population exposure for human health research: a case study of ozone in the Northern Georgia Region of the United States

Ambient monitors are commonly used to estimate exposure for epidemiological studies, and air quality modeling is infrequently applied. However air quality modeling systems have the potential to alleviate some, although not all, of the limitations of monitoring networks. To investigate this application, exposure estimates were generated for a case study high ozone episode in the Northern Georgia Region of the United States based on measurements and concentration estimates from an air quality modeling system. Hourly estimates for 2268 4-km by 4-km gridcells were generated in a domain that includes only eight ozone monitors. Individual and population-based ozone exposures were estimated using multiple approaches, including area-weighted average of modeled estimates, nearest monitor, and spatial interpolation by inverse distance weighting and kriging. Results based on concentration fields from the air quality modeling system revealed spatial heterogeneity that was obscured by approaches based on the monitoring network. With some techniques, such as spatial interpolation, monitoring data alone was insufficient to estimate exposure for certain areas, especially for rural populations. For locations far from ozone monitors, the estimates from the nearest monitor approach tended to overestimate exposure, compared to modeled estimates. Counties in which one or more monitors were present had statistically higher population density and modeled ozone estimates than did counties without monitors (p-value <0.05). This work demonstrates the use of air quality modeling to generate higher spatial and temporal resolution exposure estimates, and compares the advantages of this approach to traditional methods that use monitoring data alone. The air quality modeling method faces its own limitations, such as the need to thoroughly evaluate concentration estimates and the use of ambient levels rather than personal exposure.     

Linking high resolution mass spectrometry data with exposure and toxicity forecasts to advance high-throughput environmental monitoring

There is a growing need in the field of exposure science for monitoring methods that rapidly screen environmental media for suspect contaminants. Measurement and analysis platforms, based on high resolution mass spectrometry (HRMS), now exist to meet this need. Here we describe results of a study that links HRMS data with exposure predictions from the U.S. EPA's ExpoCast™ program and in vitro bioassay data from the U.S. interagency Tox21 consortium. Vacuum dust samples were collected from 56 households across the U.S. as part of the American Healthy Homes Survey (AHHS). Sample extracts were analyzed using liquid chromatography time-of-flight mass spectrometry (LC–TOF/MS) with electrospray ionization. On average, approximately 2000 molecular features were identified per sample (based on accurate mass) in negative ion mode, and 3000 in positive ion mode. Exact mass, isotope distribution, and isotope spacing were used to match molecular features with a unique listing of chemical formulas extracted from EPA's Distributed Structure-Searchable Toxicity (DSSTox) database. A total of 978 DSSTox formulas were consistent with the dust LC–TOF/molecular feature data (match score ≥ 90); these formulas mapped to 3228 possible chemicals in the database. Correct assignment of a unique chemical to a given formula required additional validation steps. Each suspect chemical was prioritized for follow-up confirmation using abundance and detection frequency results, along with exposure and bioactivity estimates from ExpoCast and Tox21, respectively. Chemicals with elevated exposure and/or toxicity potential were further examined using a mixture of 100 chemical standards. A total of 33 chemicals were confirmed present in the dust samples by formula and retention time match; nearly half of these do not appear to have been associated with house dust in the published literature. Chemical matches found in at least 10 of the 56 dust samples include Piperine, N,N-Diethyl-m-toluamide (DEET), Triclocarban, Diethyl phthalate (DEP), Propylparaben, Methylparaben, Tris(1,3-dichloro-2-propyl)phosphate (TDCPP), and Nicotine. This study demonstrates a novel suspect screening methodology to prioritize chemicals of interest for subsequent targeted analysis. The methods described here rely on strategic integration of available public resources and should be considered in future non-targeted and suspect screening assessments of environmental and biological media.