Poly- and perfluoroalkyl substances in maternal serum: Method development and application in Pilot Study of the Japan Environment and Children's Study

Nakayama, Shoji F.; Isobe, Takeshi; Iwai-Shimada, Miyuki; Kobayashi, Yayoi; Nishihama, Yukiko; Taniguchi, Yu; Sekiyama, Makiko; Michikawa, Takehiro; Yamazaki, Shin; Nitta, Hiroshi; Oda, Masako; Mitsubuchi, Hiroshi; Sanefuji, Masafumi; Ohga, Shouichi; Mise, Nathan; Ikegami, Akihiko; Suga, Reiko; Shimono, Masayuki

doi:10.1016/j.chroma.2020.460933

Cited by 19 publications

(13 citation statements)

References 44 publications

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“…Several methods have been developed for the quantitation of different chemical classes of PFASs in human serum and plasma, by implementing liquid chromatography coupled with tandem mass spectrometry as a suitable analytical technique for high sensitivity and selectivity. Before injection, plasma and serum samples are usually treated to remove proteins [41][42][43][44][45] and/or purified with solid-phase extraction (SPE) [16,[46][47][48][49][50][51][52][53][54][55][56][57][58]. However, only a few methods considered the emerging compounds HFPO-DA [16,43,44], F-53B 1 3 [16,53,56], DONA [16,43], or PFECHS [43,45].…”

Section: Introductionmentioning

confidence: 99%

Development and validation of an LC–MS/MS method for the quantitation of 30 legacy and emerging per- and polyfluoroalkyl substances (PFASs) in human plasma, including HFPO-DA, DONA, and cC6O4

et al. 2021

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Per-and polyfluoroalkyl substances (PFASs) include persistent organic pollutants whose spread is still ubiquitous. Efforts to substitute substances of high concern with fluorinated alternatives, such as HFPO-DA (GenX), DONA (ADONA), and cC6O4, have been made. The aim of this work was to develop and validate an isotopic dilution liquid chromatographytandem mass spectrometry (LC-MS/MS) method suitable to quantify 30 PFASs in human plasma. Analytes included legacy PFASs (PFOA, PFOS, and PFHxS), fluorinated alternatives (PFBA, PFBS, 6:2 FTSA, HFPO-DA, DONA, and cC6O4), and newly identified compounds (F-53B and PFECHS). The sample preparation was rapid and consisted of simple protein precipitation and centrifugation. Calibration standards and quality control solutions were prepared with a human pooled plasma containing relatively low background levels of the considered analytes. A complete validation was carried out: the lower limits of quantitation (LLOQs) ranged from 0.009 to 0.245 µg/L; suitable linearity (determination coefficients, R 2 0.989-0.999), precision (2.0-19.5%, relative standard deviation), and accuracy (87.9-113.1% of theoretical) were obtained for considered concentration ranges. No significant variations of analyte responses were recorded under investigated storage conditions and during matrix effect tests. The external verification confirmed the accuracy of the method, although limited to 12 analytes. The method was also applied to 38 human plasma samples to confirm its applicability. The developed assay is suitable for large-scale analyses of a wide range of legacy and emerging PFASs in human plasma. To our knowledge, this is the first published method including cC6O4 for human biomonitoring.

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Section: Introductionmentioning

confidence: 99%

Development and validation of an LC–MS/MS method for the quantitation of 30 legacy and emerging per- and polyfluoroalkyl substances (PFASs) in human plasma, including HFPO-DA, DONA, and cC6O4

et al. 2021

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“…As expected, these detection limits are considerably lower than previous CE methods coupled to UV detection (LOD ∼ 3300 nM), 39 as well as NACE methods with online sample preconcentration using large‐volume sample stacking or field‐amplified sample injections (LOD ∼ 30–280 nM) 41 . Yet, LC‐MS/MS methods with pre‐column SPE reported significantly lower LODs for PFASs ranging from 0.02 to 0.20 nM due to the much larger sample volumes injected on‐column (∼100‐fold) as compared to CE (∼10 nL) 34,38 . For these reasons, off‐line sample enrichment was critical to enable quantification of low nanomolar levels of PFOSs from serum extracts when using MSI‐CE‐MS/MS.…”

Section: Resultsmentioning

confidence: 60%

“…Analytical methods for PFAS determination require exquisite sensitivity and selectivity without complicated sample workup or background/matrix interferences 33 . Liquid chromatography coupled to tandem mass spectrometry (LC‐MS/MS) with multiple reaction monitoring (MRM) is the gold standard for analysis of nanomolar levels of PFAS in complex biological and environmental samples 16,34,35 . Standardized protocols have been developed for reliable PFAS analysis by LC‐MS/MS following pre‐column sample enrichment and off‐line clean‐up using ion‐pair extraction or anion‐exchange solid‐phase extraction (SPE) 34,36,37 .…”

Section: Introductionmentioning

confidence: 99%

Rapid biomonitoring of perfluoroalkyl substance exposures in serum by multisegment injection‐nonaqueous capillary electrophoresis‐tandem mass spectrometry

Hum

Britz‐McKibbin

2020

Analytical Science Advances

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Perfluoroalkyl substances (PFASs) are a major contaminant class due to their ubiquitous prevalence, persistence, and putative endocrine disrupting activity that may contribute to chronic disease risk notably with exposures early in life. Herein, multisegment injection-nonaqueous capillary electrophoresis-tandem mass spectrometry (MSI-NACE-MS/MS) is introduced as a high throughput approach for PFAS screening in serum samples following a simple methyl-tert-butyl ether (MTBE) liquid extraction. Separation and ionization conditions were optimized to quantify low nanomolar concentration levels of perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) from serum extracts when using multiple reaction monitoring under negative ion mode conditions. Multiplexed separations of PFOA and PFOS were achieved with excellent throughput (<3 min/sample), adequate concentration sensitivity (LOD ∼ 20 nM, S/N = 3) and good technical precision over three consecutive days of analysis (mean CV = 9.1%, n = 84). Accurate quantification of PFASs was demonstrated in maternal serum samples (n = 16) when using MSI-CE-MS/MS following pre-column sample enrichment with median concentrations of 3.46 nM (0.7-9.0 nM) and 3.29 nM (1.5-6.6 nM) for PFOA and PFOS, respectively. This was lower than average PFAS exposures measured in pregnant women who had serum collected prior to 2009 likely due to subsequent phase out of their production. Overall, this method offers a convenient approach for large-scale biomonitoring of environmental exposures to legacy PFASs and their emerging replacements that is relevant to maternal health and chronic disease risk assessment in children.

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“…Participants of the JECS pilot study were registered from February 2009 to March 2010 in four regional centers, namely, Jichi Medical University, University of Occupational and Environmental Health, Kyushu University, and Kumamoto University [15]. For the 453 participants who provided consent, maternal whole blood and cord blood samples were collected in the second to third trimester and at birth, respectively.…”

Section: Study Participants and Blood Collectionmentioning

confidence: 99%

Comparison of Simultaneous Quantitative Analysis of Methylmercury and Inorganic Mercury in Cord Blood Using LC-ICP-MS and LC-CVAFS: The Pilot Study of the Japan Environment and Children’s Study

Iwai-Shimada

Kobayashi

Isobe

et al. 2021

Toxics

Self Cite

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Prenatal exposure to methylmercury (MeHg) affects child development after birth. However, many epidemiological studies have evaluated total mercury levels without analyzing speciation. Biomonitoring of MeHg and inorganic mercury (IHg) is essential to reveal each exposure level. In this study, we compared a high-throughput analysis for mercury speciation in blood using liquid chromatography-inductively coupled plasma-mass spectrometry (LC-ICP-MS) and liquid chromatography-cold vapor atomic fluorescence spectrometry (LC-CVAFS). The validated LC-ICP-MS method was applied to 101 maternal blood and 366 cord blood samples in the pilot study of the Japan Environment and Children’s Study (JECS). The accuracy of the LC-CVAFS method ranged 90–115% determined by reference material analysis. To evaluate the reliability of 366 cord blood samples, fifty cord blood samples were randomly selected and analyzed using LC-CVAFS. The median (5th–95th percentile) concentrations of MeHg and IHg were 5.4 (1.9–15) and 0.33 (0.12–0.86) ng/mL, respectively, in maternal blood, and 6.3 (2.5–15) and 0.21 (0.08–0.49) ng/mL, respectively, in cord blood. Inter-laboratory comparison showed a relatively good agreement between LC-ICP-MS and LC-CVAFS. The median cord blood:maternal blood ratios of MeHg and IHg were 1.3 and 0.5, respectively. By analyzing speciation, we could focus on the health effects of each chemical form.

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Poly- and perfluoroalkyl substances in maternal serum: Method development and application in Pilot Study of the Japan Environment and Children's Study

Cited by 19 publications

References 44 publications

Development and validation of an LC–MS/MS method for the quantitation of 30 legacy and emerging per- and polyfluoroalkyl substances (PFASs) in human plasma, including HFPO-DA, DONA, and cC6O4

Development and validation of an LC–MS/MS method for the quantitation of 30 legacy and emerging per- and polyfluoroalkyl substances (PFASs) in human plasma, including HFPO-DA, DONA, and cC6O4

Rapid biomonitoring of perfluoroalkyl substance exposures in serum by multisegment injection‐nonaqueous capillary electrophoresis‐tandem mass spectrometry

Comparison of Simultaneous Quantitative Analysis of Methylmercury and Inorganic Mercury in Cord Blood Using LC-ICP-MS and LC-CVAFS: The Pilot Study of the Japan Environment and Children’s Study

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