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Assessing the longitudinal trend of POP concentrations in humans using high-throughput sample preparation methods developed for low-volume samples
Örebro University, School of Science and Technology.
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Human exposure to anthropogenic persistent organic pollutants (POPs) and their related effects on human health widely vary from person to person, making population-based risk assessment difficult.

This thesis aimed to evaluate how individual changes and implemented re-strictions in POP production influenced human exposure. High-throughput sample preparation methods were developed and applied to plasma samples col-lected for an epidemiological study so that the longitudinal change in concen-trations of a broad range of chlorinated (Cl), brominated (Br) and fluorinated POPs in humans could be efficiently evaluated.

Two 96-well plate extraction methods were used to determine the concentra-tions of Cl/Br POPs and fluorinated POPs in 150μL of plasma samples collected for the Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) study. Plasma samples from 1,016 men and women were collected three times between 2001 and 2014, after participants turned 70, 75 and 80 years old. Dif-ferences in longitudinal trends were observed between Cl/Br POPs and fluori-nated POPs as a result of their differences in time of production and imple-mented restrictions in use. The five year trend in 17 Cl POPs (14 polychlorinated biphenyls and 3 organochlorine pesticides), detected in the majority of the co-hort, and a tetra-brominated diphenyl ether detected in 34% of the follow-up samples showed a significant decrease in plasma concentrations. However, the change in Cl/Br POP concentrations was found to be slower in those who lost more weight and had greater increases in plasma lipids, and showed a faster decline in men versus women. The 8 perfluoroalkyl substances (PFASs) detected in the majority of the cohort showed an overall increase in PFHxS, PFNA, PFDA, and PFUnDA, while PFHpA, PFOA, FOSA, and L-PFOS showed a de-crease over ten years. One of the PFASs that showed an overall increasing trend was heavily influenced by the percentage of PFAS-contaminated drinking water distributed to the residential area.

The developed and applied methods showed a high-throughput with precise and consistent results using small sample amounts and the longitudinal trend of POPs in a prospective cohort was efficiently produced. Important information was gained on how residential location, physiological differences and changes, and implemented restrictions in POP production has effected human trends.

Place, publisher, year, edition, pages
Örebro: Örebro University , 2018. , p. 65
Series
Örebro Studies in Chemistry, ISSN 1651-4270 ; 21
Keywords [en]
Longitudinal trends; human biomonitoring; POPs; PFASs; high-throughput solid phase extraction; high-resolution mass spectrometry; tandem mass spectrometry
National Category
Other Chemistry Topics
Identifiers
URN: urn:nbn:se:oru:diva-63390ISBN: 978-91-7529-226-7 (print)OAI: oai:DiVA.org:oru-63390DiVA, id: diva2:1166574
Public defence
2018-02-16, Örebro universitet, Hörsalen, Musikhögskolan, Fakultetsgatan 1, Örebro, 09:15 (Swedish)
Opponent
Supervisors
Available from: 2017-12-15 Created: 2017-12-15 Last updated: 2018-01-24Bibliographically approved
List of papers
1. Changes in serum levels of perfluoroalkyl substances during a 10-year follow-up period in a large population-based cohort
Open this publication in new window or tab >>Changes in serum levels of perfluoroalkyl substances during a 10-year follow-up period in a large population-based cohort
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2016 (English)In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 95, p. 86-92Article in journal (Refereed) Published
Abstract [en]

Poly- and perfluoroalkyl substances (PFASs) are a group of man-made fluorinated chemicals which have, at background levels, been associated with negative health effects in humans. Thus far, most human biomonitoring studies have evaluated the general change in PFAS concentration over time by continuously testing various individuals. This is one of the few studies to report the longitudinal trend of a range of PFAS concentrations in humans. In addition, this is the first known longitudinal study to include a large background level exposed cohort of both men and women with the same age and location who were repeatedly sampled from 2001 to 2014.

The longitudinal change in concentration of eight PFASs detected in serum collected from the Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) cohort were determined and compared to results from general population studies. The sex-dependent changes in PFAS concentrations over time were also assessed.

Serum was sampled from the same individuals at ages 70 (collection period 2001-2004), 75 (2006-2009) and 80 (2011-2014,). Eight (C6-11) of fourteen (C4-13) analyzed PFASs were usually detected in over 75% of individuals and assessed using a random effects (mixed) model.

In the 579 individuals attending all three examinations, PFOSA and PFOS concentrations significantly decreased, while the remaining six PFASs significantly increased between ages 70 and 75. However, between ages 75 and 80 all PFAS concentrations significantly decreased. Overall from age 70 to 80, concentrations of PFHxS, PFUnDA, PFNA, and PFDA showed a significant increase (7% to 34%), whereas concentrations of PFOSA, PFHpA, PFOS, and PFOA (-75% to -27%) significantly decreased. Over time PFHxS concentrations increased more among women, while PFHpA concentrations showed a greater decrease among men.

From age 70 to age 80, spanning from 2001-2004 to 2011-2014, the PIVUS cohort showed decreases in circulating levels of some PFASs phased out of production with the exception of PFHxS and C>8 PFASs. Contrary to other studies, PFHxS concentrations showed the greatest overall increase, which is likely attributed to a local drinking water contamination incident.

Place, publisher, year, edition, pages
Oxford, United Kingdom: Elsevier, 2016
Keywords
Perfluoroalkyl substances, PFASs, perfluoroalkyl acids, longitudinal trends, human serum, biomonitoring
National Category
Occupational Health and Environmental Health
Identifiers
urn:nbn:se:oru:diva-51743 (URN)10.1016/j.envint.2016.08.002 (DOI)000384789500010 ()27542758 (PubMedID)2-s2.0-84992116107 (Scopus ID)
Funder
Swedish Research Council, K2009-64X-21031-01-3Swedish Research Council Formas, 216-2007-2047
Available from: 2016-08-23 Created: 2016-08-23 Last updated: 2018-07-16Bibliographically approved
2. The effect of drinking water contaminated with perfluoroalkyl substances on a 10-year longitudinal trend of plasma levels in an elderly Uppsala cohort
Open this publication in new window or tab >>The effect of drinking water contaminated with perfluoroalkyl substances on a 10-year longitudinal trend of plasma levels in an elderly Uppsala cohort
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2017 (English)In: Environmental Research, ISSN 0013-9351, E-ISSN 1096-0953, Vol. 159, p. 95-102Article in journal (Refereed) Published
Abstract [en]

BACKGROUND: In 2012, drinking water contaminated with per- and polyfluoroalkyl substances (PFASs), foremost perfluorooctanesulfonic acid (PFOS) and perfluorohexanesulfonic acid (PFHxS) at levels over 20ng/L and 40ng/L, respectively, was confirmed in Uppsala, Sweden.

OBJECTIVES: We assessed how a longitudinally sampled cohort's temporal trend in PFAS plasma concentration was influenced by their residential location and determined the plausible association or disparity between the PFASs detected in the drinking water and the trend in the study cohort.

METHODS: The Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) cohort provided plasma samples three times from 2001 to 2014. Individuals maintaining the same zip code throughout the study (n = 399) were divided into a reference (no known PFAS exposure), low, intermediate and high exposure area depending on the proportion of contaminated drinking water received. Eight PFASs detected in the majority (75%) of the cohort's plasma samples were evaluated for significant changes in temporal PFAS concentrations using a random effects (mixed) model.

RESULTS: PFHxS plasma concentrations continued to significantly increase in individuals living in areas receiving the largest percentage of contaminated drinking water (p < 0.0001), while PFOS showed an overall decrease. The temporal trend of other PFAS plasma concentrations did not show an association to the quality of drinking water received.

CONCLUSIONS: The distribution of contaminated drinking water had a direct effect on the trend in PFHxS plasma levels among the different exposure groups, resulting in increased concentrations over time, especially in the intermediate and high exposure areas. PFOS and the remaining PFASs did not show the same relationship, suggesting other sources of exposure influenced these PFAS plasma trends.

Place, publisher, year, edition, pages
Academic Press, 2017
Keywords
Perfluoroalkyl substances, Drinking water, Longitudinal trend, PIVUS cohort, Perfluorohexane sulfonic acid
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-61461 (URN)10.1016/j.envres.2017.07.050 (DOI)000413280500011 ()28780137 (PubMedID)2-s2.0-850267812292-s2.0-85026781229 (Scopus ID)
Funder
Swedish Research Council, VR; K2009-64X-21031-01-3Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning, FORMAS; 216-2007-2047
Available from: 2017-10-13 Created: 2017-10-13 Last updated: 2018-08-06Bibliographically approved
3. A new method for analysis of marker POPs in low-volume plasma and serum samples using 96-well plate solid phase extraction
Open this publication in new window or tab >>A new method for analysis of marker POPs in low-volume plasma and serum samples using 96-well plate solid phase extraction
(English)Manuscript (preprint) (Other academic)
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:oru:diva-64493 (URN)
Available from: 2018-01-24 Created: 2018-01-24 Last updated: 2018-01-24Bibliographically approved
4. Longitudinal changes in persistent organic pollutants (POPs) over 5 years in a sample of elderly men and women
Open this publication in new window or tab >>Longitudinal changes in persistent organic pollutants (POPs) over 5 years in a sample of elderly men and women
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(English)Manuscript (preprint) (Other academic)
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:oru:diva-64494 (URN)
Available from: 2018-01-24 Created: 2018-01-24 Last updated: 2018-01-24Bibliographically approved

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