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Mullin, L. G., Katz, D. R., Riddell, N., Plumb, R., Burgess, J. A., Yeung, L. W. Y. & Ericson Jogsten, I. (2019). Analysis of hexafluoropropylene oxide-dimer acid (HFPO-DA) by liquid chromatography-mass spectrometry (LC-MS): Review of current approaches and environmental levels. TrAC. Trends in analytical chemistry, 118, 828-839
Open this publication in new window or tab >>Analysis of hexafluoropropylene oxide-dimer acid (HFPO-DA) by liquid chromatography-mass spectrometry (LC-MS): Review of current approaches and environmental levels
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2019 (English)In: TrAC. Trends in analytical chemistry, ISSN 0165-9936, E-ISSN 1879-3142, Vol. 118, p. 828-839Article, review/survey (Refereed) Published
Abstract [en]

Emerging per- and polyfluorinated compounds (PFAS) compounds are of increasing interest for environmental monitoring, one being hexafluoropropylene oxide-dimer acid (HFPO-DA), commonly referred to as GenX. The following review describes existing liquid chromatography-mass spectrometry (LC-MS) methods used to analyse HFPO-DA, including sample preparation and method sensitivity relative to other PFAS. Analytical challenges are also described, in particular the significant formation of in-source fragmentation, dimer and dimer adducts which detract from [M-H](-) signal. Lastly, detected levels of HFPO-DA in environmental and biological samples are compared across the limited number of available field exposure studies, which found several mu g/L concentrations in water samples taken near fluorochemical plant discharges.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
HFPO-DA, GenX, Negative polarity electrospray ionisation, Liquid chromatography, Mass spectrometry
National Category
Chemical Sciences
Identifiers
urn:nbn:se:oru:diva-76970 (URN)10.1016/j.trac.2019.05.015 (DOI)000486383900064 ()31501636 (PubMedID)
Note

Funding Agency:

Intramural EPA  EPA999999

Available from: 2019-10-02 Created: 2019-10-02 Last updated: 2019-10-02Bibliographically approved
Yeung, L. W. Y., Yamashita, N. & Falandysz, J. (2019). Legacy and emerging perfluorinated and polyfluorinated compounds: An update. Chemosphere, 237, Article ID UNSP 124506.
Open this publication in new window or tab >>Legacy and emerging perfluorinated and polyfluorinated compounds: An update
2019 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 237, article id UNSP 124506Article in journal, Editorial material (Other academic) Published
Place, publisher, year, edition, pages
Elsevier, 2019
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-78515 (URN)10.1016/j.chemosphere.2019.124506 (DOI)000496896700130 ()31400742 (PubMedID)2-s2.0-85073703038 (Scopus ID)
Available from: 2019-12-10 Created: 2019-12-10 Last updated: 2019-12-10Bibliographically approved
Koch, A., Kärrman, A., Yeung, L. W. Y., Jonsson, M., Ahrens, L. & Wang, T. (2019). Point source characterization of per- and polyfluoroalkyl substances (PFASs) and extractable organofluorine (EOF) in freshwater and aquatic invertebrates. Environmental Science: Processes & Impacts, 21(11), 1887-1898
Open this publication in new window or tab >>Point source characterization of per- and polyfluoroalkyl substances (PFASs) and extractable organofluorine (EOF) in freshwater and aquatic invertebrates
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2019 (English)In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1887-1898Article in journal (Refereed) Published
Abstract [en]

Major point sources of per- and polyfluoroalkyl substances (PFASs) cause ubiquitous spread of PFASs in the environment. In this study, surface water and aquatic invertebrates at three Swedish sites impacted by PFAS point sources were characterized, using homologue, isomer and extractable organofluorine (EOF) profiling as well as estimation of bioaccumulation factors (BAFs) and mass discharge. Two sites were impacted by fire training (sites A and R) and the third by industrial runoff (site K). Mean Σ25PFASs concentration in water was 1920 ng L-1 at site R (n = 3), which was more than 20- and 10-fold higher than those from sites A and K, respectively. PFOS was the most predominant PFAS in all waters samples, constituting 29-79% of Σ25PFAS concentrations. Several branched isomers were detected and they substantially contributed to concentrations in surface water (e.g. 49-78% of ΣPFOS) and aquatic invertebrates (e.g. 15-28% of ΣPFOS). BAFs in the aquatic invertebrates indicated higher bioaccumulation for long chain PFASs and lower bioaccumulation for branched PFOS isomers compared to linear PFOS. EOF mass balance showed that Σ25target PFASs in water could explain up to 55% of EOF at site R. However, larger proportions of EOF (>92%) remained unknown in water from sites A and K. Mass discharges were for the first time estimated for EOF and revealed that high amounts of EOF (e.g. 8.2 g F day-1 at site A) could be transported by water to recipient water bodies relative to Σ25PFASs (e.g. 0.15 g day-1 at site A). Overall, we showed that composition profiling, BAFs and EOF mass balance can improve the characterization of PFASs around point sources.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2019
National Category
Oceanography, Hydrology and Water Resources Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-76827 (URN)10.1039/c9em00281b (DOI)31552402 (PubMedID)
Available from: 2019-09-30 Created: 2019-09-30 Last updated: 2019-11-20Bibliographically approved
Uwayezu, J.-N., Yeung, L. W. Y. & Bäckström, M. (2019). Sorption of PFOS isomers on goethite as a function of pH, dissolved organic matter (humic and fulvic acid) and sulfate. Chemosphere, 233, 896-904
Open this publication in new window or tab >>Sorption of PFOS isomers on goethite as a function of pH, dissolved organic matter (humic and fulvic acid) and sulfate
2019 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 233, p. 896-904Article in journal (Refereed) Published
Abstract [en]

Understanding the distribution of PFOS isomers between the aqueous phase and goethite is crucial, since it is an abundant sorbent and thus may have a large influence on the mobility of PFOS. This study was conducted to understand the effects of pH, humic acid (HA), fulvic acid (FA) and sulfate on sorption of PFOS isomers. The results will increase the understanding about what parameters may control the fate and transport of PFOS in surface and ground water.

The study was conducted by adding PFOS spiked water to a goethite slurry with different aqueous chemistry. Levels of total PFOS and PFOS isomers were quantified using an Ultra-Performance Liquid Chromatograph coupled to a triple quadrupole mass spectrometer. Results showed that sorption of PFOS was mainly dependent on pH; sorption decreased as pH increased. Presence of HA increased log K-d from 1.29 to 2.03, 1.76 to 1.92 and 1.51 to 1.96 at pH 5.50-7.50 for 3-/4-/4-PFOS, 6-/2-PFOS and L-PFOS, respectively. Changes in the aqueous chemistry also affected the behaviour of PFOS as the addition of Na2SO4 enhanced the sorption of PFOS. Results showed that L-PFOS was more readily sorbed to goethite at pH < 4.35 both in the presence and in the absence of humic or fulvic acids. At pH > 4.5 the 3-/4-/5-PFOS isomer group was more associated to goethite. Besides electrostatic interactions, which controlled the sorption of PFOS, this study indicate that the presence of dissolved humic substances in the aqueous phase enhances the sorption via hydrophobic mechanisms.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Goethite, Perfluorooctane sulfonate, Sorption, Humic substances, Electrostatic and hydrophobic interactions
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-75699 (URN)10.1016/j.chemosphere.2019.05.252 (DOI)000477691500099 ()31340417 (PubMedID)2-s2.0-85067315052 (Scopus ID)
Funder
Knowledge Foundation, 20160019
Available from: 2019-08-14 Created: 2019-08-14 Last updated: 2019-08-14Bibliographically approved
Hu, X. C., Tokranov, A. K., Liddie, J., Zhang, X., Grandjean, P., Hart, J. E., . . . Sunderland, E. M. (2019). Tap Water Contributions to Plasma Concentrations of Poly- and Perfluoroalkyl Substances (PFAS) in a Nationwide Prospective Cohort of U.S. Women. Journal of Environmental Health Perspectives, 127(6), Article ID 67006.
Open this publication in new window or tab >>Tap Water Contributions to Plasma Concentrations of Poly- and Perfluoroalkyl Substances (PFAS) in a Nationwide Prospective Cohort of U.S. Women
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2019 (English)In: Journal of Environmental Health Perspectives, ISSN 0091-6765, E-ISSN 1552-9924, Vol. 127, no 6, article id 67006Article in journal (Refereed) Published
Abstract [en]

BACKGROUND: Between 2013 and 2015, concentrations of poly- and perfluoroalkyl substances (PFAS) in public drinking water supplies serving at least six million individuals exceeded the level set forth in the health advisory established by the U.S. Environmental Protection Agency. Other than data reported for contaminated sites, no systematic or prospective data exist on the relative source contribution (RSC) of drinking water to human PFAS exposures.

OBJECTIVES: This study estimates the RSC of tap water to overall PFAS exposure among members of the general U.S.

POPULATION:

METHODS: We measured concentrations of 15 PFAS in home tap water samples collected in 1989-1990 from 225 participants in a nationwide prospective cohort of U.S. women: the Nurses' Health Study (NHS). We used a one-compartment toxicokinetic model to estimate plasma concentrations corresponding to tap water intake of PFAS. We compared modeled results with measured plasma PFAS concentrations among a subset of 110 NHS participants.

RESULTS: Tap water perfluorooctanoic acid (PFOA) and perfluorononanoic acid (PFNA) were statistically significant predictors of plasma concentrations among individuals who consumed [Formula: see text] cups of tap water per day. Modeled median contributions of tap water to measured plasma concentrations were: PFOA 12% (95% probability interval 11%-14%), PFNA 13% (8.7%-21%), linear perfluorooctanesulfonic acid (nPFOS) 2.2% (2.0%-2.5%), branched perfluorooctanesulfonic acid (brPFOS) 3.0% (2.5%-3.2%), and perfluorohexanesulfonic acid (PFHxS) 34% (29%-39%). In five locations, comparisons of PFASs in community tap water collected in the period 2013-2016 with samples from 1989-1990 indicated increases in quantifiable PFAS and extractable organic fluorine (a proxy for unquantified PFAS).

CONCLUSIONS: Our results for 1989-1990 compare well with the default RSC of 20% used in risk assessments for legacy PFAS by many agencies. Future evaluation of drinking water exposures should incorporate emerging PFAS.

Place, publisher, year, edition, pages
National Institute of Environmental Health Science, 2019
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-74653 (URN)10.1289/EHP4093 (DOI)000474528700004 ()31170009 (PubMedID)2-s2.0-85067472608 (Scopus ID)
Note

Funding Agencies:

Harvard National Institute of Environmental Health and Sciences (NIEHS) Center Grant  P30 ES000002 

NIH  CA186107  CA49449  ES021372 

NIH Superfund Research Program  P42ES027706 

Available from: 2019-06-10 Created: 2019-06-10 Last updated: 2019-11-14Bibliographically approved
Björnsdotter, M., Yeung, L. W. Y., Kärrman, A. & Ericson Jogsten, I. (2019). Ultra-Short-Chain Perfluoroalkyl Acids Including Trifluoromethane Sulfonic Acid in Water Connected to Known and Suspected Point Sources in Sweden. Environmental Science and Technology, 53(19), 11093-11101
Open this publication in new window or tab >>Ultra-Short-Chain Perfluoroalkyl Acids Including Trifluoromethane Sulfonic Acid in Water Connected to Known and Suspected Point Sources in Sweden
2019 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 53, no 19, p. 11093-11101Article in journal (Refereed) Published
Abstract [en]

Data presenting the environmental occurrence of ultra-short-chain perfluoroalkyl acids (PFAAs) are scarce and little is known about the potential sources. In this study, ultra-short-chain PFAAs were analyzed in water connected to potential point sources using supercritical fluid chromatography coupled with tandem mass spectrometry. Samples (n = 34) were collected in connection with firefighting training sites, landfills, and a hazardous waste management facility. Ultra-short-chain PFAAs were detected in all samples at concentrations up to 84 000 ng/L (∑C1-C3), representing up to 69% of the concentration of 29 per- and polyfluoroalkyl substances (PFASs). Trifluoroacetic acid (TFA), perfluoropropanoic acid (PFPrA), trifluoromethane sulfonic acid (TFMS), perfluoroethane sulfonic acid (PFEtS), and perfluoropropane sulfonic acid (PFPrS) were detected at concentrations up to 14 000, 53 000, 940, 1700, and 15 000 ng/L, respectively. Principal component analysis suggests that TFA is associated with landfills. PFPrS was associated with samples collected close to the source at all types of sites included in this study. These findings reveal the presence of high concentrations of ultra-short-chain PFAAs released into the environment from various sources and emphasize the large fraction of ultra-short-chain PFAAs to the total concentration of PFASs in water.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-76642 (URN)10.1021/acs.est.9b02211 (DOI)000488993500006 ()31496234 (PubMedID)2-s2.0-85072791157 (Scopus ID)
Funder
Swedish Research Council Formas, 2016-01284Swedish Environmental Protection Agency, 2219-16-030 2219-17-012Knowledge Foundation, 20160019
Available from: 2019-09-24 Created: 2019-09-24 Last updated: 2019-11-15Bibliographically approved
Parajulee, A., Lei, Y. D., Cao, X., McLagan, D. S., Yeung, L. W. Y., Mitchell, C. P. J. & Wania, F. (2018). Comparing winter-time herbicide behavior and exports in urban, rural, and mixed-use watersheds. Environmental Science: Processes & Impacts, 20(5), 767-779
Open this publication in new window or tab >>Comparing winter-time herbicide behavior and exports in urban, rural, and mixed-use watersheds
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2018 (English)In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 5, p. 767-779Article in journal (Refereed) Published
Abstract [en]

The presence of pesticides in streams in winter, five to six years following bans on their municipal use suggests that complicated transport behaviour, such as subsurface retention and/or accumulation of pesticides and its release during storms, could be important for understanding recovery time frames following bans or legislation that aim to reduce chemical inputs. We investigated late fall and winter dynamics of four herbicides in paired urban and rural watersheds in Toronto, Canada during rainfall and snowmelt. The range of average concentrations and loads of the sum of atrazine, metolachlor, 2,4-D and mecoprop overlapped in the two types of watersheds, with slightly higher average concentrations in the rural watershed. Relatively consistent herbicide concentration-discharge patterns (i. e. dilution) were observed in the urban sub-watersheds during rainfall, while concentration-discharge patterns were much more variable in the rural watershed. This suggests relatively uniform transport pathways across the urban sub-watersheds, compared to the rural watershed. Concentration-discharge patterns of the neutral herbicides atrazine and metolachlor were similar in both watersheds during snowmelt, though varying discharge patterns resulted in divergent timings of peak concentrations. In contrast, the acidic pesticides 2,4-D and mecoprop, which are primarily associated with urban uses, showed much more variable behavior across both watersheds and merit further investigation. Overall, this work highlights the need to consider pesticide dynamics throughout the year in order to more thoroughly assess the longterm efficacy of legislation governing their use.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2018
National Category
Analytical Chemistry Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-67271 (URN)10.1039/c7em00596b (DOI)000433191900005 ()29578561 (PubMedID)2-s2.0-85047605361 (Scopus ID)
Note

Funding Agencies:

Natural Sciences and Engineering Research Council of Canada  

FedDev Ontario  

Ontario Ministry of Research and Innovation via the Southern Ontario Water Consortium  

Ontario Graduate Scholarship  

TD Canada Trust 

Available from: 2018-06-15 Created: 2018-06-15 Last updated: 2018-06-15Bibliographically approved
Pan, Y., Zhang, H., Cui, Q., Sheng, N., Yeung, L. W. Y., Sun, Y., . . . Dai, J. (2018). Worldwide Distribution of Novel Perfluoroether Carboxylic and Sulfonic Acids in Surface Water. Environmental Science and Technology, 52(14), 7621-7629
Open this publication in new window or tab >>Worldwide Distribution of Novel Perfluoroether Carboxylic and Sulfonic Acids in Surface Water
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2018 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 52, no 14, p. 7621-7629Article in journal (Refereed) Published
Abstract [en]

Driven by increasingly stringent restrictions on long-chain per- and polyfluoroalkyl substances (PFASs), novel fluorinated compounds have emerged on the market. Here we report on the occurrences of several perfluoroalkyl ether carboxylic and sulfonic acids (PFECAs and PFESAs), including hexafluoropropylene oxide dimer and trimer acids (HFPO-DA and HFPO-TA), ammonium 4,8-dioxa-3 H-perfluorononanoate (ADONA), chlorinated polyfluorinated ether sulfonic acid (6:2 Cl-PFESA), and its hydrogen-substituted analogue (6:2 H-PFESA) in surface waters from China ( n = 106), the United States ( n = 12), the United Kingdom ( n = 6), Sweden ( n = 10), Germany ( n = 14), The Netherlands ( n = 6), and Korea ( n = 6). Results showed that HFPO-DA, HFPO-TA, and 6:2 Cl-PFESA (median = 0.95, 0.21, and 0.31 ng/L, respectively) were frequently detected in all countries, indicating ubiquitous dispersal and distribution in global surface waters. The presence of 6:2 H-PFESA was widely detected in China (detection rate > 95%) but not in any other country. Only trace levels of ADONA (0.013-1.5 ng/L) were detected in the Rhine River flowing through Germany. The estimated total riverine mass discharges of HFPO-DA, HFPO-TA, and ΣPFESAs reached 2.6, 6.0, and 4.3 ton/year in five of the major river systems in China. Our results indicated that novel PFECAs and PFESAs might become global contaminants, and future investigations are warranted.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-67005 (URN)10.1021/acs.est.8b00829 (DOI)000439397800006 ()29749740 (PubMedID)2-s2.0-85049342448 (Scopus ID)
Note

Funding Agencies:

National Natural Science Foundation of China  21737004  31320103915 

Chinese Academy of Sciences  XDB14040202 

Available from: 2018-05-24 Created: 2018-05-24 Last updated: 2018-08-02Bibliographically approved
Ericson Jogsten, I. & Yeung, L. W. Y. (2017). Analysis of ultra-short chain perfluoroalkyl substances in Swedish environmental waters. Örebro, Sweden: Örebro university
Open this publication in new window or tab >>Analysis of ultra-short chain perfluoroalkyl substances in Swedish environmental waters
2017 (English)Report (Other academic)
Abstract [en]

The purpose of this study was to investigate the environmental occurrence of ultra-short chain perfluoroalkyl substances (PFASs) in Swedish water samples. So far established protocols have focused on measuring PFASs with a carbon chain length of four or more carbons. In this study, perfluoroalkyl sulfonates of chain lengths of two, perfluoroethane sulfonate (PFEtS), and three, perfluoropropane sulfonate (PFPrS), carbons have been measured using a newly established instrumental method employing supercritical fluid separation (SFC) coupled to tandem mass spectrometry detection.

A total of 26 samples were analysed, including ground water, surface water, rain water and snow. The sample locations included military and civilian airports, a former hard chromium plating facility, the vicinity of a hazardous waste management facility and background areas (lake surface water, rain and snow). Results show that both PFPrS and PFEtS could be detected in environmental samples using SFC separation coupled to triple quadrupole detection. Out of the 26 samples analysed, the ultra-short-chain PFPrS could be detected and quantified in 22 samples. The concentrations for PFPrS in all the samples ranged between 0.93 ng/l to 39 000 ng/l. The ultra-short-chain PFPEtS could be quantified in all of the 26 samples, with a concentration range between 0.07 and 5 700 ng/l. The highest concentrations represents highly contaminated ground water samples collected from a military airport. In the samples, PFPrS had a relative contribution to total PFAS concentration of 6 and 10 %, indicating the importance of measuring these compounds in environmental samples.

Place, publisher, year, edition, pages
Örebro, Sweden: Örebro university, 2017. p. 18
Keywords
Ultra-short chain PFAS, water
National Category
Analytical Chemistry Environmental Sciences
Research subject
Chemistry; Environmental Chemistry
Identifiers
urn:nbn:se:oru:diva-64607 (URN)
Funder
Swedish Environmental Protection Agency, 2219-16-030
Available from: 2018-01-29 Created: 2018-01-29 Last updated: 2018-02-02Bibliographically approved
Joudan, S., Yeung, L. W. Y. & Mabury, S. A. (2017). Biological cleavage of the C-P bond in perfluoroalkyl phosphinic acids in male Sprague-Dawley rats and the formation of persistent and reactive metabolites. Journal of Environmental Health Perspectives, 125(11), Article ID 117001.
Open this publication in new window or tab >>Biological cleavage of the C-P bond in perfluoroalkyl phosphinic acids in male Sprague-Dawley rats and the formation of persistent and reactive metabolites
2017 (English)In: Journal of Environmental Health Perspectives, ISSN 0091-6765, E-ISSN 1552-9924, Vol. 125, no 11, article id 117001Article in journal (Refereed) Published
Abstract [en]

BACKGROUND: Perfluoroalkyl phosphinic acids (PFPiAs) have been detected in humans, wildlife, and various environmental matrices. These compounds have been used with perfluoroalkyl phosphonic acids (PFPAs) as surfactants in consumer products and as nonfoaming additives in pesticide formulations. Unlike the structurally related perfluoroalkyl sulfonic and carboxylic acids, little is known about the biological fate of PFPiAs.

OBJECTIVES: We determined the biotransformation products of PFPiAs and some pharmacokinetic parameters in a rat model.

METHODS: Male Sprague-Dawley rats received an oral gavage dose of either C6/C8PFPiA, C8/C8PFPiA, or C8PFPA. Blood was sampled over time, and livers were harvested upon sacrifice. Analytes were quantified using ultra-high-performance liquid chromatography-tandem mass spectrometry or gas chromatography-mass spectrometry.

RESULTS: PFPiAs were metabolized to the corresponding PFPAs and 1H-perfluoroalkanes (1H-PFAs), with 70% and 75% biotransformation 2 wk after a single bolus dose for C6/C8PFPiA and C8/C8PFPiA, respectively. This is the first reported cleavage of a C-P bond in mammals, and the first attempt, with a single-dose exposure, to characterize the degradation of any perfluoroalkyl acid. Elimination half-lives were 1.9±0.5 and 2.8±0.8 days for C6/C8PFPiA and C8/C8PFPiA, respectively, and 0.95±0.17 days for C8PFPA. Although elimination half-lives were not determined for 1H-PFAs, concentrations were higher than the corresponding PFPAs 48 h after rats were dosed with PFPiAs, suggestive of slower elimination.

CONCLUSIONS: PFPiAs were metabolized in Sprague-Dawley rats to form persistent PFPAs as well as 1H-PFAs, which contain a labile hydrogen that may undergo further metabolism. These results in rats produced preliminary findings of the pharmacokinetics and metabolism of PFPiAs, which should be further investigated in humans. If there is a parallel between the disposition of these chemicals in humans and rats, then humans with detectable amounts of PFPiAs in their blood may be undergoing continuous exposure.

Place, publisher, year, edition, pages
National Institute of Environmental Health Sciences (NIEHS), 2017
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-63315 (URN)10.1289/EHP1841 (DOI)000416837300004 ()29135439 (PubMedID)2-s2.0-85033388855 (Scopus ID)
Note

Funding Agency:

National Science and Engineering Research Council Discovery grant

Available from: 2017-12-12 Created: 2017-12-12 Last updated: 2017-12-19Bibliographically approved
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