Human biomonitoring of per- and polyfluoroalkyl substances in German blood plasma samples from 1982 to 2019

The findings of per- and polyfluoroalkyl substances (PFAS) in humans and the environment all over the world have raised concerns and public awareness for this group of man-made chemicals. In the last three decades, this led to different regulatory restrictions for specific PFAS as well as shifts in...

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Main Authors: Bernd Göckener, Till Weber, Heinz Rüdel, Mark Bücking, Marike Kolossa-Gehring
Format: Article
Language:English
Published: Elsevier 2020-12-01
Series:Environment International
Subjects:
Online Access:http://www.sciencedirect.com/science/article/pii/S016041202032078X
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author Bernd Göckener
Till Weber
Heinz Rüdel
Mark Bücking
Marike Kolossa-Gehring
author_facet Bernd Göckener
Till Weber
Heinz Rüdel
Mark Bücking
Marike Kolossa-Gehring
author_sort Bernd Göckener
collection DOAJ
description The findings of per- and polyfluoroalkyl substances (PFAS) in humans and the environment all over the world have raised concerns and public awareness for this group of man-made chemicals. In the last three decades, this led to different regulatory restrictions for specific PFAS as well as shifts in the production and usage of these substances. In this study, we analyzed the PFAS levels of 100 human blood plasma samples collected from 2009 to 2019 for the German Environmental Specimen Bank (ESB) to further elucidate the time course of exposure towards this substance group as shown by Schröter-Kermani et al., (2013) with samples from 1982 to 2010. A spectrum of 37 PFAS, including perfluorocarboxylic (PFCA) and –sulfonic acids (PFSA) as well as potential precursors and substitutes like ADONA, GenX or F-53B was analyzed by UHPLC coupled with high-resolution mass spectrometry. Validation was successful for 33 of the substances.The two legacy substances perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) were detected in every sample of the 2009–2019 dataset and showed the highest concentrations with ranges of 0.27–14.0 ng/mL and 1.21–14.1 ng/mL, respectively. A significant portion of total PFOS analytes was present as branched isomers (mean: 34 ± 7%). High detection frequencies of 95% and 82% were also found for perfluorohexane sulfonic acid (PFHxS) and perfluorononanoic acid (PFNA), respectively, but in lower concentrations (PFHxS: <LOQ – 4.62 ng/mL; PFNA: <LOQ – 3.66 ng/mL) than PFOA and PFOS. Besides other PFCA and PFSA only 8:2 fluorotelomer sulfonic acid (8:2 FtS) and N-methyl perfluorooctane sulfonamidoacetic acid were detected in very few samples. In combination with the previous results from 1982 to 2010, declining temporal trends were observed for all PFAS (PFOA, PFNA, PFHxS, and PFOS) frequently detected in the ESB samples. The results of this study indicate a decrease in human exposure to known PFAS in Germany over the last three decades and emphasize the importance of long-term human biomonitoring studies for investigating the effects of chemical regulation.
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spelling doaj.art-e12d45ed8f994c0d9e46a784b70eef912022-12-21T20:48:24ZengElsevierEnvironment International0160-41202020-12-01145106123Human biomonitoring of per- and polyfluoroalkyl substances in German blood plasma samples from 1982 to 2019Bernd Göckener0Till Weber1Heinz Rüdel2Mark Bücking3Marike Kolossa-Gehring4Fraunhofer Institute for Molecular Biology and Applied Ecology IME, Auf dem Aberg 1, 57392 Schmallenberg, Germany; Corresponding author.German Environment Agency (Umweltbundesamt), Corrensplatz 1, 14195 Berlin, GermanyFraunhofer Institute for Molecular Biology and Applied Ecology IME, Auf dem Aberg 1, 57392 Schmallenberg, GermanyFraunhofer Institute for Molecular Biology and Applied Ecology IME, Auf dem Aberg 1, 57392 Schmallenberg, Germany; Monash University, School of Chemistry, 13 Rainforest Walk, Clayton, Victoria 3800, AustraliaGerman Environment Agency (Umweltbundesamt), Corrensplatz 1, 14195 Berlin, GermanyThe findings of per- and polyfluoroalkyl substances (PFAS) in humans and the environment all over the world have raised concerns and public awareness for this group of man-made chemicals. In the last three decades, this led to different regulatory restrictions for specific PFAS as well as shifts in the production and usage of these substances. In this study, we analyzed the PFAS levels of 100 human blood plasma samples collected from 2009 to 2019 for the German Environmental Specimen Bank (ESB) to further elucidate the time course of exposure towards this substance group as shown by Schröter-Kermani et al., (2013) with samples from 1982 to 2010. A spectrum of 37 PFAS, including perfluorocarboxylic (PFCA) and –sulfonic acids (PFSA) as well as potential precursors and substitutes like ADONA, GenX or F-53B was analyzed by UHPLC coupled with high-resolution mass spectrometry. Validation was successful for 33 of the substances.The two legacy substances perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) were detected in every sample of the 2009–2019 dataset and showed the highest concentrations with ranges of 0.27–14.0 ng/mL and 1.21–14.1 ng/mL, respectively. A significant portion of total PFOS analytes was present as branched isomers (mean: 34 ± 7%). High detection frequencies of 95% and 82% were also found for perfluorohexane sulfonic acid (PFHxS) and perfluorononanoic acid (PFNA), respectively, but in lower concentrations (PFHxS: <LOQ – 4.62 ng/mL; PFNA: <LOQ – 3.66 ng/mL) than PFOA and PFOS. Besides other PFCA and PFSA only 8:2 fluorotelomer sulfonic acid (8:2 FtS) and N-methyl perfluorooctane sulfonamidoacetic acid were detected in very few samples. In combination with the previous results from 1982 to 2010, declining temporal trends were observed for all PFAS (PFOA, PFNA, PFHxS, and PFOS) frequently detected in the ESB samples. The results of this study indicate a decrease in human exposure to known PFAS in Germany over the last three decades and emphasize the importance of long-term human biomonitoring studies for investigating the effects of chemical regulation.http://www.sciencedirect.com/science/article/pii/S016041202032078XPFASHuman biomonitoringTemporal trendsEnvironmental specimen bankHBM4EU
spellingShingle Bernd Göckener
Till Weber
Heinz Rüdel
Mark Bücking
Marike Kolossa-Gehring
Human biomonitoring of per- and polyfluoroalkyl substances in German blood plasma samples from 1982 to 2019
Environment International
PFAS
Human biomonitoring
Temporal trends
Environmental specimen bank
HBM4EU
title Human biomonitoring of per- and polyfluoroalkyl substances in German blood plasma samples from 1982 to 2019
title_full Human biomonitoring of per- and polyfluoroalkyl substances in German blood plasma samples from 1982 to 2019
title_fullStr Human biomonitoring of per- and polyfluoroalkyl substances in German blood plasma samples from 1982 to 2019
title_full_unstemmed Human biomonitoring of per- and polyfluoroalkyl substances in German blood plasma samples from 1982 to 2019
title_short Human biomonitoring of per- and polyfluoroalkyl substances in German blood plasma samples from 1982 to 2019
title_sort human biomonitoring of per and polyfluoroalkyl substances in german blood plasma samples from 1982 to 2019
topic PFAS
Human biomonitoring
Temporal trends
Environmental specimen bank
HBM4EU
url http://www.sciencedirect.com/science/article/pii/S016041202032078X
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