The transfer of the perfluoroalkyl acids (PFAAs) perfluorobutanesulfonate (PFBS), perfluorohexanesulfonate (PFHxS), perfluorooctanesulfonate (PFOS), and perfluorooctanoate (PFOA) from feed into tissue and milk of dairy cows was investigated. Holstein cows (n = 6) were fed a PFAA-contaminated feed for 28 days. After the PFAA-feeding period, three cows were slaughtered while the others were fed PFAA-free feed for another 21 days (depuration period). For PFAA analysis plasma, liver, kidney, and muscle tissue, urine, and milk were sampled and analyzed using high-performance liquid chromatography (HPLC) with tandem mass spectrometry (MS/MS). The average daily intake of dairy cows was 3.4 ± 0.7, 4.6 ± 1.0, 7.6 ± 3.7 and 2.0 ± 1.2 μg/kg body weight (bw) for PFBS, PFHxS, PFOS, and PFOA, respectively. Overall, PFBS, PFHxS, PFOS, and PFOA showed different kinetics in dairy cows. In plasma, concentrations of PFBS (mean = 1.2 ± 0.8 μg/L) and PFOA (mean = 8.5 ± 5.7 μg/L) were low, whereas PFHxS and PFOS continuously increased during the PFAA-feeding period up to maximal concentrations of 419 ± 172 and 1903 ± 525 μg/L, respectively. PFOS in plasma remained constantly high during the depuration period. PFOS levels were highest in liver, followed by kidney, without significant differences between feeding periods. The highest PFHxS levels were detected in liver and kidney of cows slaughtered on day 29 (61 ± 24 and 98 ± 31 μg/kg wet weight (ww)). The lowest PFAA levels were detected in muscle tissue. At the end of the feeding study, cumulative secretion in milk was determined for PFOS (14 ± 3.6%) and PFHxS (2.5 ± 0.2%). The other two chemicals were barely secreted into milk: PFBS (0.01 ± 0.02%) and PFOA (0.1 ± 0.06%). Overall, the kinetics of PFOA were similar to those of PFBS and substantially differed from those of PFHxS and PFOS. The very low concentration of PFBS in plasma and milk, the relatively high urinary excretion, and only traces of PFBS in liver (0.3 ± 0.3 μg/kg ww) and kidney (1.0 ± 0.3 μg/kg ww) support the conclusion that PFBS does not accumulate in the body of dairy cows.
A pilot study was performed with dairy sheep to generate the first data on the transfer of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) from feed into food of animal origin. Corn silage was cultivated on cropland in Lower Saxony in Germany where, as a result of illegal waste disposal in 2006, farmland was contaminated with perfluorinated alkylacids (PFAAs). Two sheep were exposed by way of PFAA-contaminated corn silage to PFOS (1.16 and 1.45 μg/kg body weight [bw]/d, respectively) and PFOA (0.43 and 0.53 μg/kg bw/d) during a period of 21 days. During the PFAA-feeding period, PFOS levels in plasma increased continuously to maximum concentration of 103 and 240 μg/L for sheep 1 and sheep 2, respectively. The PFOA plasma concentration remained low (sheep 1 = 3.3 ± 2.2 μg/L; sheep 2 = 15.6 ± 8.3 μg/L). Data indicate that urinary excretion is the primary clearance route for PFOA (sheep 1 = 51 %; sheep 2 = 55 %), whereas PFOS excretion by way of urine could not be quantified. The highest PFOS excretion (4 to 5 %) was detected in faeces. PFOS was also excreted at higher levels than PFOA by way of milk. During a period of 21 days, a total PFOS transfer into milk ≤ 2 % was calculated. Overall, total excretion of PFOS was significantly lower compared with that of PFOA (PFOS 6 %; PFOA 53 to 56 %). PFOS levels in sheep 1 and sheep 2 were highest in liver (885 and 1,172 μg/kg weight wet [ww], respectively) and lowest in muscle tissue (24.4 and 35.1 μg/kg ww, respectively). PFOA levels in muscle tissue were low for sheep 2 (0.23 μg/kg ww) and not detectable after the PFAA-free feeding period in sheep 1. A slight background load of PFOS in liver (1.5 μg/kg ww) and kidney (0.3 μg/kg ww) was detected in sheep 3 (control).
The transfer of a mixture of perfluoroalkyl acids (PFAAs) from contaminated feed into the edible tissues of 24 fattening pigs was investigated. Four perfluoroalkyl sulfonic (PFSAs) and three perfluoroalkyl carboxylic acids (PFCAs) were quantifiable in feed, plasma, edible tissues, and urine. As percentages of unexcreted PFAA, the substances accumulated in plasma (up to 51%), fat, and muscle tissues (collectively, meat 40-49%), liver (under 7%), and kidney (under 2%) for most substances. An exception was perfluorooctanesulfonic acid (PFOS), with lower affinity for plasma (23%) and higher for liver (35%). A toxicokinetic model is developed to quantify the absorption, distribution, and excretion of PFAAs and to calculate elimination half-lives. Perfluorohexanoic acid (PFHxA), a PFCA, had the shortest half-life at 4.1 days. PFSAs are eliminated more slowly (e.g., half-life of 634 days for PFOS). PFAAs in pigs exhibit longer elimination half-lives than in most organisms reported in the literature, but still shorter than in humans.
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