Diet is a major source of human exposure to hazardous environmental chemicals, including many perfluoroalkyl acids (PFAAs). Several assessment methods of dietary exposure to PFAAs have been used previously, but there is a lack of comparisons between methods.
To assess human exposure to PFAAs through diet by different methods and compare the results.
We studied the dietary exposure to PFAAs in 61 Norwegian adults (74% women, average age: 42 years) using three methods: i) by measuring daily PFAA intakes through a 1-day duplicate diet study (separately in solid and liquid foods), ii) by estimating intake after combining food contamination with food consumption data, as assessed by 2-day weighted food diaries and iii) by a Food Frequency Questionnaire (FFQ). We used existing food contamination data mainly from samples purchased in Norway and if not available, data from food purchased in other European countries were used. Duplicate diet samples (n=122) were analysed by liquid chromatography coupled with tandem mass spectrometry (LC-MS/MS) to quantify 15 PFAAs (11 perfluoroalkyl carboxylates and 4 perfluoroalkyl sulfonates). Differences and correlations between measured and estimated intakes were assessed.
The most abundant PFAAs in the duplicate diet samples were PFOA, PFOS and PFHxS and the median total intakes were 5.6ng/day, 11ng/day and 0.78ng/day, respectively. PFOS and PFOA concentrations were higher in solid than liquid samples. PFOS was the main contributor to the contamination in the solid samples (median concentration 14pg/g food), while it was PFOA in the liquid samples (median concentrations: 0.72pg/g food). High intakes of fats, oils, and eggs were statistically significantly related to high intakes of PFOS and PFOA from solid foods. High intake of milk and consumption of alcoholic beverages, as well as food in paper container were related to high PFOA intakes from liquid foods. PFOA intakes derived from food diary and FFQ were significantly higher than those derived from duplicate diet, but intakes of PFOS derived from food diary and FFQ were significantly lower than those derived from duplicate diet. We found a positive and statistically significant correlation between the PFOS intakes derived from duplicate diet with those using the food diary (rho=0.26, p-value=0.041), but not with the FFQ. Additionally, PFOA intakes derived by duplicate diet were significantly correlated with estimated intakes from liquid food derived from the food diary (rho=0.34, p=0.008) and estimated intakes from the FFQ (rho=0.25, p-value=0.055).
We provide evidence that a food diary or a FFQ-based method can provide comparable intake estimates to PFOS and PFOA intakes derived from a duplicate diet study. These less burdensome methods are valuable and reliable tools to assess dietary exposure to PFASs in human studies.
Exposure to per- and polyfluoroalkyl substances through the consumption of fish from lakes affected by aqueous film-forming foam emissions - A combined epidemiological and exposure modeling approach. The SAMINOR 2 Clinical Study.
Releases of aqueous film-forming foams (AFFFs) from airport firefighting activities have been identified as important local point sources of per- and polyfluoroalkyl substances (PFASs) in nearby waterways. PFASs can be taken up by fish, and in turn by the humans that consume them. Despite the global extent of AFFF emissions, few studies exist on related impacts on humans. We aimed to investigate the associations between the consumption of fish from AFFF-affected waters and serum PFAS concentrations in humans using a combination of statistical tools, empirical data, and toxicokinetic modeling. Participants of the SAMINOR 2 Clinical Study were the basis for this study sample, which comprised 74 persons. Fifty-nine participants who reported consuming fish from AFFF-affected waters and 15 nonconsumers completed a questionnaire and gave serum samples. Participants were classified based on their consumption of trout and char: high (n=16), moderate (n=16), low (n=27), and nonconsumers (n=15); and serum samples were tested for the presence of 15 PFASs. Perfluorooctane sulfonic acid (PFOS) was found in all participants, with the highest concentrations detected in the high consumption group (geometric means, 28ng/mL) compared to the low consumption group and nonconsumers (10 and 11ng/mL, respectively). In an analysis of variance contrast model, a significant, positive increasing trend was seen for fish consumption and PFOS, perfluorohexane sulfonic acid (PFHxS), and perfluorononanoic acid (PFNA). Toxicokinetic modeling allowed us to predict the median increases in serum concentrations of PFOS, PFHxS, and PFNA among high consumers within a factor of 2.2. The combination of statistical evaluation and toxicokinetic modeling clearly demonstrated a positive relationship between consumption of fish from AFFF-affected waters and serum PFAS concentrations. Further studies on dietary exposure to other PFASs present in AFFF and its consequences on human health are warranted.
This study summarises the results of the levels of 21 perfluoroalkyl substances (PFASs) in 50 selected pooled samples representing 15 food commodities with the special focus on those of animal origin, as meat, seafood, fish, milk, dairy products and hen eggs, which are commonly consumed in various European markets, e.g. Czech, Italian, Belgian and Norwegian. A new, rapid sample preparation approach based on the QuEChERS extraction procedure was applied. Ultra-performance liquid chromatography (UHPLC) coupled to tandem mass spectrometry (MS/MS) employing electrospray ionisation (ESI) in negative mode was used for the quantification of target analytes. Method quantification limits (MQLs) were in the range of 1-10 ng kg(-1) (ng l(-1)) for fish, meat, hen eggs, cheese and milk, and in the range of 2.5-125 ng kg(-1) for butter. Only 16 of the group of 21 PFASs were found in at least one analysed sample. From 16 PFASs, perfluorooctane sulfonate (PFOS) was the most frequently detected analyte present in approximately 50% of samples (in the range of 0.98-2600 ng kg(-1)). PFCAs with C8-C14 carbon chain were presented in approximately 20% of samples. The concentration ranges of individual compounds in the respective groups of PFASs were: 2.33-76.3 ng kg(-1) for PFSAs (without PFOS), 4.99-961 ng kg(-1) for PFCAs, 10.6-95.4 ng kg(-1) for PFPAs, and 1.61-519 ng kg(-1) for FOSA. The contamination level in the analysed food commodities decreased in the following order: seafood > pig/bovine liver > freshwater/marine fish > hen egg > meat > butter. When comparing the total contamination and profiles of PFASs in food commodities that originated from various sampling countries, differences were identified, and the contents decreased as follows: Belgium > Norway, Italy > Czech Republic.
In this study, contamination levels were determined for polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and perfluorinated alkylated substances (PFASs) in traditional Greenland seafood items, such as raw and smoked fish fillet (salmon and halibut), whale and seal meat and narwhal mattak (skin and blubber). The daily intake of PCBs, PBDEs and PFASs through traditional seafood items in Greenland was assessed. Based on the presented levels of contaminants, in combination with earlier food intake studies, suggests that the daily exposure was below the tolerable daily intake threshold for all compounds. BDE-47 was the only PBDE-congener detected in all food items, except in smoked halibut. The levels of BDE-47 varied from