•This study contributed to the field of human exposure to poly- and perfluoroalkyl substances.•Dietary exposure from the ingestion of food and drinks was the predominant exposure pathway.•Measured ...and modelled serum concentrations were in the same order of magnitude.•The estimated daily intakes of PFASs in this study were lower than the health-based guidance values.
Exposure to PFASs may result in adverse health effects. This study aimed to characterise the exposure to PFASs from diet, house dust, indoor air, and dermal contact and the relative contribution from different external exposure pathways to human serum concentrations. Daily intakes of 18 perfluoroalkyl acids (PFAAs) and 12 PFAA precursors from diet, dust ingestion, inhalation of indoor air and dermal absorption were estimated using a comprehensive dataset comprising 61 adults from the Oslo area, Norway. Concentrations of PFAAs and PFAA precursors in house dust, indoor air, hand wipes, foods and drinks were utilised to estimate the daily intakes. Perfluorooctanesulfonate (PFOS) was the predominant PFAS in serum for this study group. On a median level, perfluorooctanoate (PFOA) contributed most to the total estimated daily intake of PFAAs, with a median intake of 280 (range: 72–1810) pg·kg bw−1·day−1, covering both direct and indirect (precursors) exposure. Out of this, only 3% (range: <1–48%) of the total PFOA intake came from indirect exposure. Dietary exposure from ingestion of food and drinks was in general the predominant exposure pathway, followed by exposure from ingestion of house dust, inhalation of indoor air, and dermal absorption, but considerable variations were observed among individuals. House dust ingestion and indoor air inhalation contributed most to the total intakes for some participants, for which most of them were among the 20% participants with the highest total estimated intakes. Some statistical significant associations between concentrations of PFASs measured in serum and estimated intakes were observed. Measured serum concentrations and modelled serum concentrations based on external exposure estimates were in the same order of magnitude for PFOS, PFHxS, PFOA, and PFNA, but only PFOA concentrations were comparable, 1.9 and 2.0 ng mL−1 for observed and modelled serum concentrations, respectively. The estimated daily intakes of PFASs in this study were lower than the health-based guidance values, e.g. the tolerable weekly intakes derived by EFSA. This study underlines the importance of performing studies considering multiple exposure pathways on an individual basis.
The worldwide ban of several formulations of brominated flame retardants has caused an increase in the production of organophosphorus flame retardants (PFRs) to meet the existing fire regulations for ...a wide range of household products. This biomonitoring study surveys the occurrence of the metabolites from PFRs and related plasticizers (dialkyl and diaryl phosphates; DAPs) in urine from a Norwegian mother–child cohort (48 mothers and 54 children). Concentrations of DAPs were higher in the children than in their mothers (Wilcoxon signed-rank test p=0.001). Median urinary concentrations of diphenyl phosphate (DPHP) were 1.1 and 0.51ng/mL in children and mothers, respectively, followed by bis(1,3-dichloro-2-propyl) phosphate (BDCIPP) with medians of 0.23 and 0.12ng/mL, respectively. Detection frequencies for bis(2-butoxyethyl) phosphate (BBOEP) in urine from children and mothers were 32 and 1%, respectively (median<0.18ng/mL), and for di-n-butyl phosphate (DNBP) 15 and 8%, respectively (median<0.12ng/mL). The concentrations of DPHP and BDCIPP in urine from children were significantly correlated with those found for their parent compounds in air and dust from the households (Spearman's rank correlations 0.30<Rs<0.36; p<0.05). For mothers, only the urinary concentration of BDCIPP was correlated to its precursor in dust from the households (Rs=0.40; p<0.01), which might indicate higher impact of the household environment on children than mothers. A diurnal variability study of the mothers' urinary concentrations of DPHP and BDCIPP showed lower concentrations at time periods when women were likely to be outside the household. In contrast, no relevant associations between organophosphate metabolites in urine and food consumption data obtained through a 24hour recall were seen. This suggests that the residential environment is a more important exposure pathway to PFRs than the diet.
•Urinary concentrations of BDCIPP and DPHP were higher for children than for mothers.•Concentrations of metabolites in urine correlated with organophosphates in dust and air.•Exposure of children to organophosphates can be related to indoor environment.•Diet seems to play a minor role for exposure to organophosphate flame retardants.•Morning urine reflects well the 24hour average excretion of BDCIPP and DPHP.
This study investigates the occurrence of 37 organohalogen and organophosphate flame retardants (FRs) from Norwegian households (n = 48) and classrooms from two primary schools (n = 6). Around 80% of ...the targeted FRs were detected in air and dust from the sampling sites. The comparison of settled dust with floor dust revealed no statistical differences between median concentrations of the FRs (n = 12). Decabromodiphenyl ether and tris(2-butoxyethyl) phosphate showed the highest median floor dust concentrations in both environments. In the air samples, the highest concentrations were observed for 2,2′,4,4′-tetrabromodiphenyl ether and tris(1-chloro-2-propyl) phosphate. Remarkably, the emerging FR, 4-(1,2-dibromoethyl)-1,2-dibromocyclohexane, abbreviated as TBECH or DBE-DBCH, showed the highest indoor air concentrations reported in the literature (households, 77.9 pg/m3 and schools, 46.6 pg/m3). Good Spearman correlations between the FR concentrations in dust and air (0.36 < R < 0.76) showed that is possible to estimate the concentrations in air from analyzed dust, or vice versa. Sources and pathways of exposure to FRs were assessed for the households. The main findings were that frequent vacuum cleaning resulted in lower FR concentrations in dust and that dermal contact with dust, for both children and mothers, was as important for the intake of organophosphate FRs as dust ingestion.
Fifty-seven pooled archived human serum samples were analyzed to assess the time trends as well as influence of age and gender on selected perfluorinated compounds (PFCs) in Norwegian residents. The ...study comprised determinations of 19 PFCs in serum samples pooled according to year of collection from 28 years in the period 1976 to 2007. A 9-fold increase in the serum concentrations of perfluorooctyl sulfonate, perfluorooctanoic acid, and perfluoroheptyl sulfonate was measured for men (40−50 years) from 1977 to the mid 1990s where the concentrations reached a plateau before starting to decrease around year 2000. A similar trend was also seen for perfluorohexyl sulfonate, perfluorononanoic acid, perfluorodecanoic acid, and perfluoroundecanoic acid, but no clear decline was observed for these PFCs in the recent years. No statistically significant difference was observed between the PFC levels in the male and female serum pools, though the statistical power is low due to few data points. For most PFCs, the concentrations in the human serum samples were found to increase with age in the pools from 2007, while the results for 1976, 1987, and 1998 were more varying. Several PFCs were significantly intercorrelated.
Per- and polyfluorinated compounds (PFCs) have been found to be ubiquitously distributed in human populations, however the sources of human exposure are not fully characterized. A wide range of PFCs ...were determined in paired samples of indoor air and dust from 41 Norwegian households. Up to 18 ionic and 9 neutral PFCs were detected. The concentrations found are comparable to or lower than what has previously been reported in North America, Europe, and Asia. The highest median concentrations in dust were observed for perfluorohexanoic acid (28 ng/g), perfluorononanoic acid (23 ng/g), perfluorododecanoic acid (19 ng/g), and perfluorooctanoic acid (18 ng/g). However, perfluoroalkyl sulfonic acids (PFSAs) were also frequently detected. Fluortelomer alcohols were the most prominent compounds found in indoor air, with median concentrations for 8:2 fluortelomer alcohol, 10:2 fluortelomer alcohol, and 6:2 fluortelomer alcohol of 5173, 2822, and 933 pg/m3 air, respectively. All perfluoroalkyl sulfonamides and sulfonamidoethanols (FOSA/FOSEs) were detected in more than 40% of the air samples. For the first time, significant positive correlations (p < 0.05) between PFSAs in house dust and FOSA/FOSEs in the indoor air have been shown, supporting the hypothesis that FOSA/FOSEs may be transformed to PFSAs. Further, we found the age of the residence to be a predictor of PFC concentrations in both indoor air and house dust. These results are important for estimating the exposure to PFCs from the indoor environment and for characterization of exposure pathways.
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•The EU Horizon 2020 project HBM4EU targets seven substance groups and two metals.•Best suitable exposure biomarkers, matrices and analytical methods were suggested.•The selection was ...based on generally applicable criteria, e.g. method sensitivity.•Some conflicts were identified between the criteria and common exposure biomarkers.•Stringent quality assurance and control measures should be included and reported.
The major purpose of human biomonitoring is the mapping and assessment of human exposure to chemicals. The European initiative HBM4EU has prioritized seven substance groups and two metals relevant for human exposure: Phthalates and substitutes (1,2-cyclohexane dicarboxylic acid diisononyl ester, DINCH), bisphenols, per- and polyfluoroalkyl substances (PFASs), halogenated and organophosphorous flame retardants (HFRs and OPFRs), polycyclic aromatic hydrocarbons (PAHs), arylamines, cadmium and chromium. As a first step towards comparable European-wide data, the most suitable biomarkers, human matrices and analytical methods for each substance group or metal were selected from the scientific literature, based on a set of selection criteria. The biomarkers included parent compounds of PFASs and HFRs in serum, of bisphenols and arylamines in urine, metabolites of phthalates, DINCH, OPFRs and PAHs in urine as well as metals in blood and urine, with a preference to measure Cr in erythrocytes representing Cr (VI) exposure. High performance liquid chromatography-tandem mass spectrometry (LC-MS/MS) was the method of choice for bisphenols, PFASs, the HFR hexabromocyclododecane (HBCDD), phenolic HFRs as well as the metabolites of phthalates, DINCH, OPFRs and PAHs in urine. Gas chromatographic (GC) methods were selected for the remaining compounds, e.g. GC-low resolution MS with electron capture negative ionization (ECNI) for HFRs. Both GC–MS and LC-MS/MS were suitable for arylamines. New developments towards increased applications of GC–MS/MS may offer alternatives to GC–MS or LC-MS/MS approaches, e.g. for bisphenols. The metals were best determined by inductively coupled plasma (ICP)-MS, with the particular challenge of avoiding interferences in the Cd determination in urine. The evaluation process revealed research needs towards higher sensitivity and non-invasive sampling as well as a need for more stringent quality assurance/quality control applications and assessments.
Harmonized data describing simultaneous exposure to a large number of environmental contaminants in-utero and during childhood is currently very limited.
To characterize concentrations of a large ...number of environmental contaminants in pregnant women from Europe and their children, based on chemical analysis of biological samples from mother-child pairs.
We relied on the Early-Life Exposome project, HELIX, a collaborative project across six established population-based birth cohort studies in Europe. In 1301 subjects, biomarkers of exposure to 45 contaminants (i.e. organochlorine compounds, polybrominated diphenyl ethers, per- and polyfluoroalkyl substances, toxic and essential elements, phthalate metabolites, environmental phenols, organophosphate pesticide metabolites and cotinine) were measured in biological samples from children (6–12 years) and their mothers during pregnancy, using highly sensitive biomonitoring methods.
Most of the exposure biomarkers had high detection frequencies in mothers (35 out of 45 biomarkers with >90% detected) and children (33 out of 45 biomarkers with >90% detected). Concentrations were significantly different between cohorts for all compounds, and were generally higher in maternal compared to children samples. For most of the persistent compounds the correlations between maternal and child concentrations were moderate to high (Spearman Rho > 0.35), while for most non-persistent compounds correlations were considerably lower (Spearman Rho < 0.15). For mercury, PFOS and PFOA a considerable proportion of the samples of both mothers and their children exceeded the HBM I value established by The Human Biomonitoring Commission of the German Federal Environment Agency.
Although not based on a representative sample, our study suggests that children across Europe are exposed to a wide range of environmental contaminants in fetal life and childhood including many with potential adverse effects. For values exceeding the HBM I value identification of specific sources of exposure and reducing exposure in an adequate way is recommended. Considerable variability in this “chemical exposome” was seen between cohorts, showing that place of residence is a strong determinant of one's personal exposome. This extensive dataset comprising >100,000 concentrations of environmental contaminants in mother-child pairs forms a unique possibility for conducting epidemiological studies using an exposome approach.
•Children across Europe are exposed to a wide range of environmental contaminants.•Considerable variability in the “chemical exposome” was seen between cohorts.•Significant differences in concentrations between mothers and children were found.
Phthalates and bisphenol A (BPA) are ubiquitous in our environment. These chemicals have been characterized as endocrine disruptors that can cause functional impairment of development and ...reproduction. Processed and packaged foods are among the major sources of human exposure to these chemicals. No previous report showing the levels of these chemicals in food items purchased in Norway is available. The aim of the present study was to determine the concentration of ten different phthalates and BPA in foods and beverages purchased on the Norwegian market and estimate the daily dietary exposure in the Norwegian adult population. Commonly consumed foods and beverages in Norway were purchased in a grocery store and analysed using gas- and liquid chromatography coupled with mass spectrometry. Daily dietary exposures to these chemicals in the Norwegian adult population were estimated using the latest National dietary survey, Norkost 3 (2010–2011). This study showed that phthalates and BPA are found in all foods and beverages that are common to consume in Norway. The detection frequency of phthalates in the food items varied from 11% for dicyclohexyl phthalate (DCHP) to 84% for di-iso-nonyl phthalate (DiNP), one of the substitutes for bis(2-ethylhexyl) phthalate (DEHP). BPA was found in 54% of the food items analysed. Among the different phthalates, the highest concentrations were found for DEHP and DiNP in the food items. Estimated dietary exposures were also equally high and dominated by DEHP and DiNP (400–500ng/kg body weight (bw)/day), followed by di-iso-butyl phthalate (DiBP), di-n-butyl phthalate (DnBP), di-n-octyl phthalate (DnOP) and di-iso-decyl phthalate (DiDP) (30–40ng/kg bw/day). Dimethyl phthalate (DMP), diethylphthalate (DEP) and DCHP had the lowest concentrations and the exposures were around 10–20ng/kg bw/day. Estimated dietary exposure to BPA was 5ng/kg bw/day. In general, levels of phthalates and BPA in foods and beverages from the Norwegian market are comparable to other countries worldwide. Grain and meat products were the major contributors of exposure to these chemicals in the Norwegian adult population. The estimated dietary exposures to these chemicals were considerably lower than their respective tolerable daily intake (TDI) values established by the European Food Safety Authority (EFSA).
•Ten phthalates and bisphenol A were determined in food items bought in Norway.•Concentrations were highest for phthalates DEHP and DiNP.•Grain and meat products were major contributors to these chemicals in Norway.•Estimated dietary exposures were lower than respective tolerable daily intakes.
Pregnant women and children are especially vulnerable to exposures to food contaminants, and a balanced diet during these periods is critical for optimal nutritional status.
Our objective was to ...study the association between diet and measured blood and urinary levels of environmental contaminants in mother-child pairs from six European birth cohorts (
mothers and 1,288 children).
We assessed the consumption of seven food groups and the blood levels of organochlorine pesticides, polybrominated diphenyl ethers, polychlorinated biphenyls (PCBs), per- and polyfluoroalkyl substances (PFAS), and heavy metals and urinary levels of phthalate metabolites, phenolic compounds, and organophosphate pesticide (OP) metabolites. Organic food consumption during childhood was also studied. We applied multivariable linear regressions and targeted maximum likelihood based estimation (TMLE).
Maternal high (
) versus low (
) fish consumption was associated with 15% higher PCBs geometric mean (GM)
; 95% confidence interval (CI): 1.02, 1.29, 42% higher perfluoroundecanoate (PFUnDA) (
; 95% CI: 1.20, 1.68), 89% higher mercury (Hg) (
; 95% CI: 1.47, 2.41) and a 487% increase in arsenic (As) (
; 95% CI: 2.57, 9.23) levels. In children, high (
) versus low (
) fish consumption was associated with 23% higher perfluorononanoate (PFNA) (
; 95% CI: 1.08, 1.40), 36% higher PFUnDA (
; 95% CI: 1.12, 1.64), 37% higher perfluorooctane sulfonate (PFOS) (
; 95% CI: 1.22, 1.54), and
higher Hg and As
(95% CI: 1.91, 4.31) and
(95% CI: 2.23, 3.21) concentrations. Using TMLE analysis, we estimated that fish consumption within the recommended 2-3 times/week resulted in lower PFAS, Hg, and As compared with higher consumption. Fruit consumption was positively associated with OP metabolites. Organic food consumption was negatively associated with OP metabolites.
Fish consumption is related to higher PFAS, Hg, and As exposures. In addition, fruit consumption is a source of exposure to OPs. https://doi.org/10.1289/EHP5324.
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•A multi-chemical evaluation of 60 breast milk samples was performed.•31 organic contaminants and 14 toxic and essential elements were determined.•Breastfed babies are exposed to a ...mixture of hazardous chemicals.•Maternal features (age, body mass index) and smoking are key exposure factors.•Breast milk from low-income mothers has higher levels of DDT and DDE.
Breastfeeding is one of the most effective ways to ensure child health and survival, with several benefits for both the infants and their mothers. However, breast milk can contain environmental pollutants with endocrine disruption capacity, neurotoxicity and/or potential to alter microbiota. Monitoring breast milk provides information on the current chemical exposure of breastfed infants and, in addition, on the current and historical exposure of nursing mothers. In this study, the levels of a wide range of pollutants were measured in breast milk of Spanish nursing mothers. Target chemicals were dichlorodiphenyltrichloroethane (DDT), dichlorodiphenyldichloroethylene (DDE), hexachlorobenzene (HCB), oxy-chlordane, polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), per- and poly-fluoroalkyl substances (PFASs) (including perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA)), chlorpyrifos, bisphenol A (BPA), tetrabromobisphenol A (TBBPA), and a number of toxic and essential elements. Traces of most chemicals were found. A correlation between the levels of some persistent organic pollutants (POPs) and maternal characteristics (age and body mass index) was observed, while smoking was associated to higher concentrations of some toxic elements. Higher levels of PCBs were detected in samples from Spanish primiparous mothers compared to non-Spanish multiparous women. Breast milk from low-income mothers showed higher content of DDT and DDE than high-income mothers. Although breastfeeding is clearly beneficial for babies, the exposure to this mixture of hazardous substances, as well as their interaction and combined effects must not be disregarded.
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