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  • 1. Du, Xinyu
    et al.
    Yuan, Bo
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Zhou, Yihui
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Qiu, Yanling
    Yin, Ge
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Zhao, Jianfu
    Short-, Medium-, and Long-Chain Chlorinated Paraffins in Wildlife from Paddy Fields in the Yangtze River Delta2018In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 52, no 3, p. 1072-1080Article in journal (Refereed)
    Abstract [en]

    Short-chain chlorinated paraffins (SCCPs) were added to Annex A of the Stockholm Convention on Persistent Organic Pollutants in April, 2017. As a consequence of this regulation, increasing production and usage of alternatives, such as medium- and long-chain chlorinated paraffins (MCCPs and LCCPs, respectively), is expected. Little is known about the environmental fate and behavior of MCCPs and LCCPs. In the present study, SCCPs, MCCPs, and LCCPs were analyzed in nine wildlife species from paddy fields in the Yangtze River Delta, China, using atmospheric pressure chemical ionization-quadrupole time-of-flight mass spectrometry. SCCPs, MCCPs, and LCCPs were detected in all samples at concentrations ranging from <91-43000, 96-33 000, and 14-10000 ng/g lipid, respectively. Most species contained primarily MCCPs (on average 44%), with the exception of collared scops owl and common cuckoo, in which SCCPs (43%) accumulated to a significantly (i.e., p < 0.05) greater extent than MCCPs (40%). Cl-6 groups were dominant in most species except for yellow weasel and short-tailed mamushi, which contained primarily Cl-7 groups. Principal components analysis, together with CP concentrations and carbon stable isotope analysis showed that habitat and feeding habits were key factors driving CP accumulation and congener group patterns in wildlife. This is the first report of LCCP exposure in wildlife and highlights the need for data on risks associated with CP usage.

  • 2. Gyllenhammar, Irina
    et al.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sandblom, Oskar
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Berger, Urs
    Ahrens, Lutz
    Lignell, Sanna
    Wiberg, Karin
    Glynn, Anders
    Perfluoroalkyl Acids (PFAAs) in Serum from 2-4-Month-Old Infants: Influence of Maternal Serum Concentration, Gestational Age, Breast-Feeding, and Contaminated Drinking Water2018In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 52, no 12, p. 7101-7110Article in journal (Refereed)
    Abstract [en]

    Little is known about factors influencing infant perfluorinated alkyl acid (PFAA) concentrations. Associations between serum PFAA concentrations in 2-4-month-old infants (n = 101) and determinants were investigated by multiple linear regression and general linear model analysis. In exclusively breastfed infants, maternal serum PFAA concentrations 3 weeks after delivery explained 13% (perfluoroundecanoic acid, PFUnDA) to 73% (perfluorohexanesulfonate, PFHxS) of infant PFAA concentration variation. Median infant/maternal ratios decreased with increasing PFAA carbon chain length from 2.8 for perfluoroheptanoic acid and perfluorooctanoic acid (PFOA) to 0.53 for PFUnDA and from 1.2 to 0.69 for PFHxS and perfluorooctanesulfonate (PFOS). Infant PFOA, perfluorononanoic acid (PFNA), and PFOS levels increased 0.7-1.2% per day of gestational age. Bottle-fed infants had mean concentrations of PFAAs 2 times lower than and a mean percentage of branched (%br) PFOS isomers 1.3 times higher than those of exclusively breast-fed infants. PFOA, PFNA, and PFHxS levels increased 8-11% per week of exclusive breast-feeding. Infants living in an area receiving PFAA-contaminated drinking water had 3-fold higher mean perfluorobutanesulfonate (PFBS) and PFHxS concentrations and higher mean %br PFHxS. Prenatal PFAA exposure and postnatal PFAA exposure significantly contribute to infant PFAA serum concentrations, depending on PFAA carbon chain length. Moderately PFBS- and PFHxS-contaminated drinking water is an important indirect exposure source.

  • 3. Gyllenhammar, Irina
    et al.
    Diderholm, Barbro
    Gustafsson, Jan
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Helmholtz Centre for Environmental Research – UFZ, Germany.
    Ridefelt, Peter
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Lignell, Sanna
    Lampa, Erik
    Glynn, Anders
    Perfluoroalkyl acid levels in first-time mothers in relation to offspring weight gain and growth2018In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 111, p. 191-199Article in journal (Refereed)
    Abstract [en]

    We investigated if maternal body burdens of perfluoroalkyl acids (PFAAs) at the time of delivery are associated with birth outcome and if early life exposure (in utero/nursing) is associated with early childhood growth and weight gain. Maternal PFAA body burdens were estimated by analysis of serum samples from mothers living in Uppsala County, Sweden (POPUP), sampled three weeks after delivery between 1996 and 2011. Data on child length and weight were collected from medical records and converted into standard deviation scores (SDS). Multiple linear regression models with appropriate covariates were used to analyze associations between maternal PFAA levels and birth outcomes (n = 381). After birth Generalized Least Squares models were used to analyze associations between maternal PFAA and child growth (n = 200). Inverse associations were found between maternal levels of perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA), and perfluoroundecanoic acid (PFUnDA), and birth weight SDS with a change of - 0.10 to - 0.18 weight SDS for an inter-quartile range (IQR) increase in ng/g PFAA. After birth, weight and length SDS were not significantly associated with maternal PFAA. However, BMI SDS was significantly associated with PFOA, PFNA, and PFHxS at 3 and 4 years of age, and with PFOS at 4 and 5 years of age. If causal, these associations suggest that PFAA affects fetal and childhood body development in different directions.

  • 4. Huang, Susie S. Y.
    et al.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. AXYS Analytical Services Ltd., Canada.
    Chandramouli, Bharat
    Butler, Heather
    Helbing, Caren C.
    Cosgrove, John R.
    Xenobiotics Produce Distinct Metabolomic Responses in Zebrafish Larvae (Danio rerio)2016In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 50, no 12, p. 6526-6535Article in journal (Refereed)
    Abstract [en]

    Sensitive and quantitative protocols for characterizing low-dose effects are needed to meet the demands of 21st century chemical hazard assessment. To test the hypothesis that xenobiotic exposure at environmentally relevant concentrations produces specific biochemical fingerprints in organisms, metabolomic perturbations in zebrafish (Danio rerio) embryo/larvae were measured following 24 h exposures to 13 individual chemicals covering a wide range of contaminant classes. Measured metabolites (208 in total) included amino acids, biogenic amines, fatty acids, bile acids, sugars, and lipids. The 96-120 h post-fertilization developmental stage was the most appropriate model for detecting xenobiotic-induced metabolomic perturbations. Metabolomic fingerprints were largely chemical- and dose-specific and were reproducible in multiple exposures over a 16-month period. Furthermore, chemical-specific responses were detected in the presence of an effluent matrix; importantly, in the absence of morphological response. In addition to improving sensitivity for detecting biological responses to low-level xenobiotic exposures, these data can aid the classification of novel contaminants based on the similarity of metabolomic responses to well-characterized model compounds. This approach is clearly of use for rapid, sensitive, and specific analyses of chemical effect on organisms, and can supplement existing methods, such as the Zebrafish Embryo Toxicity assay (OECD TG236), with molecular-level information.

  • 5. Huang, Susie S. Y.
    et al.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Veldhoen, Nik
    Chandramouli, Bharat
    Butler, Heather
    Helbing, Caren C.
    Cosgrove, John R.
    A multi-omic approach to elucidate low-dose effects of xenobiotics in zebrafish (Danio rerio) larvae2017In: Aquatic Toxicology, ISSN 0166-445X, E-ISSN 1879-1514, Vol. 182, p. 102-112Article in journal (Refereed)
    Abstract [en]

    Regulatory-approved toxicity assays_such as the OECD Fish Embryo Toxicity Assay (TG236) allow correlation of chemical exposure to adverse morphological phenotypes. However, these assays are ineffective in assessing sub-lethal (i.e. low-dose) effects, or differentiating between similar phenotypes induced by different chemicals. Inclusion of multi-omic analyses in studies investigating xenobiotic action provides improved characterization of biological response, thereby enhancing prediction of toxicological outcomes in whole animals in the absence of morphological effects. In the current study, we assessed perturbations in both the metabolome and transcriptome of zebrafish (Danio rerio; ZF) larvae exposed from 96 to 120 h post fertilization to environmental concentrations of acetaminophen (APAP), diphenhydramine (DH), carbamazepine (CBZ), and fluoxetine (FLX); common pharmaceuticals with known mechanisms of action. Multi-omic responses were evaluated independently and integrated to identify molecular interactions and biological relevance of the responses. Results indicated chemical-and dose-specific changes suggesting differences in the time scale of transcript abundance and metabolite production. Increased impact on the metabolome relative to the transcriptome in FLX-treated animals suggests a stronger post-translational effect of the treatment. In contrast, the transcriptome showed higher sensitivity to perturbation in DH-exposed animals. Integration of `omic' responses using multivariate approaches provided additional insights not obtained by independent `omic' analyses and demonstrated that the most distinct overall response profiles were induced following low-dose exposure for all 4 pharmaceuticals. Importantly, changes in transcript abundance corroborated with predictions from metabolomic enrichment analyses and the identified perturbed biological pathways aligned with known xenobiotic mechanisms of action. This work demonstrates that a multi-omic toxicological approach, coupled with a sensitive animal model such as ZF larvae, can help characterize the toxicological relevance of acute low-dose chemical exposures.

  • 6.
    Löfstedt Gilljam, John
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Leonel, Juliana
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Is Ongoing Sulfluramid Use in South America a Significant Source of Perfluorooctanesulfonate (PFOS)? Production Inventories, Environmental Fate, and Local Occurrence2016In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 50, no 2, p. 653-659Article in journal (Refereed)
    Abstract [en]

    Despite international phase-out initiatives, production and use of perfluorooctanesulfonate (PFOS) and related substances continues in some countries. In Brazil, the PFOS-precursor N-ethyl perfluorooctane sulfonamide (EtFOSA) is used in Sulfluramid, a pesticide for controlling leaf-cutting ants. New data on production, environmental fate, and occurrence of Brazilian Sulfluramid are reported herein. From 2003 to 2013, Brazilian Sulfluramid manufacturing increased from 30 to 60 tonnes yr(-1) EtFOSA. During this time <1.3 tonnes yr(-1) were imported, while exports increased from similar to 0.3 to 2 tonnes yr(-1). From 2004 to 2015, most EtFOSA was exported to Argentina (7.2 tonnes), Colombia (2.07 tonnes), Costa Rica (1.13 tonnes), Equador (2.16 tonnes), and Venezuela (2.4 tonnes). Within Brazil, sales occurred primarily in the states of Minas Gerais, Sao Paulo, Mato Grosso do Sul, Espirito Santo, and Bahia. Model simulations predict EtFOSA will partition to soils, while transformation products perfluorooctane sulfonamide (FOSA) and PFOS are sufficiently mobile to leach into surface waters. In support of these predictions, up to 3400 pg L(-)1 of FOSA and up to 1100 pg L(-)1 of PFOS were measured in Brazilian surface water, while EtFOSA was not detected. The high FOSA/PFOS ratio observed here (up to 14:1) is unprecedented in the scientific literature to our knowledge. Depending on the extent of conversion of EtFOSA, cumulative Brazilian Sulfluramid production and import from 2004 to 2015 may contribute between 167 and 487 tonnes of PFOS/FOSA to the environment. These levels are clearly nontrivial and of concern since production is continuing unabated.

  • 7. Nascimento, Rodrigo A.
    et al.
    Nunoo, Deborah B. O.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Bizkarguenaga, Ekhine
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Schultes, Lara
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Zabaleta, Itsaso
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of the Basque Country (UPV/EHU), Spain.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Spanó, Saulo
    Leonel, Juliana
    Sulfluramid use in Brazilian agriculture: A source of per- and polyfluoroalkyl substances (PFASs) to the environment2018In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 242, p. 1436-1443Article in journal (Refereed)
    Abstract [en]

    N-Ethyl perfluorooctane sulfonamide (EtFOSA) is a perfluorooctane sulfonate (PFOS) precursor and the active ingredient in sulfluramid, a pesticide which is used extensively in Brazil for management of leaf cutting ants. Here we investigate the occurrence of EtFOSA, PFOS, and other per- and polyfluoroalkyl substances (PFASs) in soil, eucalyptus leaves, water (ground, riverine, and coastal (estuarine/marine)) and coastal sediment from an agricultural region of Bahia State, Brazil. This area contains a larger number of eucalyptus plantations where sulfluramid is suspected to be applied. Soil, leaves, and coastal water (marine/estuarine) contained Sigma PFAS concentrations of up to 5400 pg g(-1), 979 pg g(-1), and 1020 pg L-1, respectively, with PFAS profiles generally dominated by PFOS and perfluorooctane sulfonamide (FOSA). Coastal sediment contained Sigma PFAS concentrations of up to 198 pg g(-1), with PFOS, FOSA, and perfluorooctanoic acid (PFOA) being the most frequently observed PFASs. These substances are all potential EtFOSA transformation products, pointing to sulfluramid as a possible source. In riverine water, Sigma PFAS concentrations of up to 8930 pg L-1 were observed. PFOS and PFOA were detected in all river water samples. Groundwater also exhibited PFAS contamination (5730 pg L-1 EPFAS5), likely from sulfluramid use. The observation of other PFASs (e.g. perfluorobutanoic acid) in freshwater suggests that other PFAS sources (in addition to sulfluramid) may be important in this region. Overall, these data support the hypothesis that sulfluramid use contributes to the occurrence of PFASs in the Brazilian environment.

  • 8. Nyberg, Elisabeth
    et al.
    Awad, Raed
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Bignert, Anders
    Ek, Caroline
    Sallsten, Gerd
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Inter-individual, inter-city, and temporal trends of per- and polyfluoroalkyl substances in human milk from Swedish mothers between 1972 and 20162018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 8Article in journal (Refereed)
    Abstract [en]

    Inter-individual, inter-city, and temporal trends of 19 per- and polyfluoroalkyl substances (PFASs) were investigated in human milk collected in Stockholm (1972-2016) and Gothenburg (2007-2015), Sweden. The concentrations of perfluorohexane sulfonate (PFHxS), perfluorononanoate (PFNA), perfluorodecanoate (PFDA), perfluoroundecanoate (PFUnDA), and perfluorotridecanoate (PFTrDA) in human milk from Stockholm increased significantly over the entire monitoring periods, whereas branched (Br) and linear (L) isomers of perfluorooctane sulfonamide (FOSA) decreased. In human milk from Gothenburg, significant downward trends were detected for perfluorododecanoate (PFDoDA), PFHxS and Br-perfluorooctane sulfonate (Br-PFOS) over the last decade. This declining trend was also observed for perfluorohexanoate (PFHxA), PFHxS, perfluorooctanoate (PFOA) and Br-PFOS in Stockholm over the same time period. No significant differences were observed in concentrations or relative PFAS profiles between Stockholm and Gothenburg. However, a comparison of the PFAS profile in Stockholm milk revealed distinct profiles for the time periods 1972-1996, 2000-2012, and 2013-2016, reflecting a shift in exposure over time. The lower bound estimated daily intake (EDI) for Sigma PFAS concentrations in infants ranged from 7.1-40 ng per kg body weight per day (ng/kg bw/d) in Stockholm and from 5.2-25 ng/kg bw/d in Gothenburg over the studied time period, consistent with other European countries. Overall these data indicate that exposure to some legacy PFASs via breastmilk is declining, presumably as a result of regulation and phase-out initiatives. However, increasing concentrations for other PFASs and a shift in the overall PFAS profile in recent years may pose an ongoing health risk to infants.

  • 9.
    Plassmann, Merle M.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Fischer, Stellan
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Nontarget Time Trend Screening in Human Blood2018In: Environmental Science and Technology Letters, E-ISSN 2328-8930, Vol. 5, no 6, p. 335-340Article in journal (Refereed)
    Abstract [en]

    Human biomonitoring (HBM) programs monitor exposure to a limited number of prioritized chemicals resulting in some important substances being overlooked. Nontarget analysis shows promise for capturing novel substances, yet the large quantity of data produced by these methods remains challenging to interrogate. Here, we apply a prioritization strategy for temporal nontarget HBM data, which shortlists features with increasing time trends, possibly representing substances which are bioaccumulating or to which humans are increasingly exposed. Human whole blood sampled in Germany between 1983 and 2015 was extracted using a modified QuEChERS method and analyzed by UHPLC-Oribtrap-mass spectrometry. Following alignment, peak detection, grouping, and gap filling, up to 14,460 features were obtained. This number was reduced to <= 716 using time trend ratios and Spearman's rank correlation coefficients to identify features which increased over the 32-year time series. Increasing features were investigated further using the KemI market list database (which prioritizes based on human hazard and/or exposure potential) as well as data-dependent product ion scans, followed by MetFrag and mzCloud database searches. Finally, seven prioritized substances, including one pharmaceutical, two pesticides, and four performance chemicals, were confirmed using standards, demonstrating the potential of time trend screening as a prioritization strategy for nontarget HBM data.

  • 10.
    Plassmann, Merle M.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Tengstrand, Erik
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Åberg, K. Magnus
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Non-target time trend screening: a data reduction strategy for detecting emerging contaminants in biological samples2016In: Analusis, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 408, no 16, p. 4203-4208Article in journal (Refereed)
    Abstract [en]

    Non-targeted mass spectrometry-based approaches for detecting novel xenobiotics in biological samples are hampered by the occurrence of naturally fluctuating endogenous substances, which are difficult to distinguish from environmental contaminants. Here, we investigate a data reduction strategy for datasets derived from a biological time series. The objective is to flag reoccurring peaks in the time series based on increasing peak intensities, thereby reducing peak lists to only those which may be associated with emerging bioaccumulative contaminants. As a result, compounds with increasing concentrations are flagged while compounds displaying random, decreasing, or steady-state time trends are removed. As an initial proof of concept, we created artificial time trends by fortifying human whole blood samples with isotopically labelled standards. Different scenarios were investigated: eight model compounds had a continuously increasing trend in the last two to nine time points, and four model compounds had a trend that reached steady state after an initial increase. Each time series was investigated at three fortification levels and one unfortified series. Following extraction, analysis by ultra performance liquid chromatography high-resolution mass spectrometry, and data processing, a total of 21,700 aligned peaks were obtained. Peaks displaying an increasing trend were filtered from randomly fluctuating peaks using time trend ratios and Spearman's rank correlation coefficients. The first approach was successful in flagging model compounds spiked at only two to three time points, while the latter approach resulted in all model compounds ranking in the top 11 % of the peak lists. Compared to initial peak lists, a combination of both approaches reduced the size of datasets by 80-85 %. Overall, non-target time trend screening represents a promising data reduction strategy for identifying emerging bioaccumulative contaminants in biological samples.

  • 11.
    Posselt, Malte
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Jaeger, Anna
    Schaper, Jonas L.
    Radke, Michael
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Determination of polar organic micropollutants in surface and pore water by high-resolution sampling-direct injection-ultra high performance liquid chromatography-tandem mass spectrometry2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 12, p. 1716-1727Article in journal (Refereed)
    Abstract [en]

    Hyporheic zones (HZs) are dynamic and complex transition regions between rivers and aquifers which are thought to play an important role in the attenuation of environmental micropollutants. Non-steady state and small-scale hyporheic processes which affect micropollutants in the HZ are poorly characterized due to limitations in existing analytical methodologies. In this work we developed a method for high spatio-temporal resolution analysis of polar organic micropollutants (POMs) in hyporheic pore- and surface waters by combining (semi-) automatic low volume sampling techniques with direct-injection ultra-high performance liquid chromatography tandem mass spectrometry. The method is capable of quantifying 25 parent compounds and 18 transformation products (TPs) using only 0.4 mL of water and few preparation steps. Application of the method to both surface and pore water revealed significant (i.e. > an order of magnitude) differences in POM concentrations over small time and spatial scales (i.e. < a few hours and tens of cm, respectively). Guanylurea, a TP of the antidiabetic drug metformin was detected at unprecedentedly high concentrations. Collectively, this method is suitable for in situ characterization of POMs at high spatial and temporal resolution and with minimal disturbance of natural flow paths and infiltration of surface water.

  • 12. Reardon, Anthony J. F.
    et al.
    Karathra, Jacqueline
    Ribbenstedt, Anton
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    MacDonald, Amy M.
    Kinniburgh, David W.
    Hamilton, Trevor J.
    Fouad, Karim
    Martin, Jonathan W.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of Alberta, Canada.
    Neurodevelopmental and Metabolomic Responses from Prenatal Coexposure to Perfluorooctanesulfonate (PFOS) and Methylmercury (MeHg) in Sprague-Dawley Rats2019In: Chemical Research in Toxicology, ISSN 0893-228X, E-ISSN 1520-5010, Vol. 32, no 8, p. 1656-1669Article in journal (Refereed)
    Abstract [en]

    Methylmercury (MeHg) and perfluoro-octanesulfonate (PFOS) are major contaminants of human blood that are both common in dietary fish, thereby raising questions about their combined impact on human development. Here, pregnant Sprague-Dawley rats ingested a daily dose, from gestational day 1 through to weaning, of either 1 mg/kg bw PFOS (PFOS-only), 1 mg/kg MeHg (MeHg-only), a mixture of 0.1 mg/kg PFOS and 1 mg/kg MeHg (Low-Mix), or of 1 mg/kg of PFOS and 1 mg/kg MeHg (High-Mix). Newborns were monitored for physical milestones and reflexive developmental responses, and in juveniles the spontaneous activity, anxiety, memory, and cognition were assessed. Targeted metabolomics of 199 analytes was applied to sectioned brain regions of juvenile offspring. Newborns in the High-Mix group had decreased weight gain as well as delayed reflexes and innate behavioral responses compared to controls and individual chemical groups indicating a toxicological interaction on early development. In juveniles, cumulative mixture effects increased in a dose-dependent manner in tests of anxiety-like behavior. However, other developmental test results suggested antagonism, as PFOS-only and MeHg-only juveniles had increased hyperactivity and thigmotaxic behavior, respectively, but fewer effects in Low-Mix and High-Mix groups. Consistent with these behavioral observations, a pattern of antagonism was also observed in neurochemicals measured in rat cortex, as PFOS-only and MeHg-only juveniles had altered concentrations of metabolites (e.g., lipids, amino acids, and biogenic amines), while no changes were evident in the combined exposures. The cortical metabolites altered in PFOS-only and MeHg-only exposed groups are involved in inhibitory and excitatory neurotransmission. These proof-of-principle findings at relatively high doses indicate the potential for toxicological interaction between PFOS and MeHg, with developmental-stage specific effects. Future mixture studies at lower doses are warranted, and prospective human birth cohorts should consider possible confounding effects from PFOS and mercury exposure on neurodevelopment.

  • 13.
    Ribbenstedt, Anton
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Ziarrusta, Haizea
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of the Basque Country (UPV/EHU), Spain.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Development, characterization and comparisons of targeted and non-targeted metabolomics methods2018In: PLoS ONE, ISSN 1932-6203, E-ISSN 1932-6203, Vol. 13, no 11, article id e0207082Article in journal (Refereed)
    Abstract [en]

    The potential of a metabolomics method to detect statistically significant perturbations in the metabolome of an organism is enhanced by excellent analytical precision, unequivocal identification, and broad metabolomic coverage. While the former two metrics are usually associated with targeted metabolomics and the latter with non-targeted metabolomics, a systematic comparison of the performance of both approaches has not yet been carried out. The present work reports on the development and performance evaluation of separate targeted and non-targeted metabolomics methods. The targeted approach facilitated determination of 181 metabolites (quantitative analysis of 18 amino acids, 11 biogenic amines, 5 neurotransmitters, 5 nucleobases and semi-quantitative analysis of 50 carnitines, 83 phos-phatidylcholines, and 9 sphingomyelins) using ultra-performance liquid chromatography - tandem mass spectrometry (UPLC-MS/MS) and flow injection-tandem mass spectrometry (Fl-MS/MS). Method accuracy and/or precision were assessed using replicate samples of NIST SRM1950 as well as fish liver and brain tissue from Gilthead Bream (Sparus aurata). The non-target approach involved UPLC-high resolution (Orbitrap) mass spectrometry (UPLC-HRMS). Testing of ionization mode and stationary phase revealed that a combination of positive electrospray ionization and HILIC chromatography produced the largest number of chromatographic features during non-target analysis. Furthermore, an evaluation of 4 different sequence drift correction algorithms, and combinations thereof, revealed that batchCorr produced the best precision in almost every test. However, even following correction of non-target data for signal drift, the precision of targeted data was better, confirming our existing assumptions about the strengths of targeted metabolomics. Finally, the accuracy of the online MS2-library mzCloud was evaluated using reference standards for 38 different metabolites. This is among the few studies that have systematically evaluated the performance of targeted and non-targeted metabolomics and provides new insight into the advantages and disadvantages of each approach.

  • 14.
    Schellenberger, Steffen
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Jönsson, Christina
    Mellin, Pelle
    Levenstam, Oscar
    liagkouridis, Ioannis
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Ribbenstedt, Anton
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Hanning, Anne-Charlotte
    Schultes, Lara
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Persson, Caiza
    Plassmann, Merle
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Benskin, Jonathan
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Release of side-chain fluorinated polymer-containing microplastic fibers from functional textiles during washing and first estimates of perfluoroalkyl acid emissionsIn: Article in journal (Refereed)
  • 15.
    Schultes, Lara
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Peaslee, Graham F.
    Brockman, John D.
    Majumdar, Ashabari
    McGuinness, Sean R.
    Wilkinson, John T.
    Sandblom, Oskar
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Ngwenyama, Ruth A.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Total Fluorine Measurements in Food Packaging: How Do Current Methods Perform?2019In: Environmental Science and Technology Letters, E-ISSN 2328-8930, Vol. 6, no 2, p. 73-78Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFASs) represent a class of more than 4000 compounds. Their large number and structural diversity pose a considerable challenge to analytical chemists. Measurement of total fluorine in environmental samples and consumer products is therefore critical for rapidly screening for PFASs and for assessing the fraction of unexplained fluorine(i.e., fluorine mass balance). Here we compare three emerging analytical techniques for total fluorine determination: combustion ion chromatography (CIC), particle-induced gamma-ray emission spectroscopy (PIGE), and instrumental neutron activation analysis (INAA). Application of each method to a certified reference material (CRM), spiked filters, and representative food packaging samples revealed good accuracy and precision. INAA and PIGE had the advantage of being nondestructive, while CIC displayed the lowest detection limits. Inconsistencies between the methods arose due to the high aluminum content in the CRM, which precluded its analysis by INAA, and sample heterogeneity (i.e., coating on the surface of the material), which resulted in higher values from the surface measurement technique PIGE compared to the values from the bulk volume techniques INAA and CIC. Comparing CIC-based extractable organic fluorine to target PFAS measurements of food packaging samples by liquid chromatography-tandem mass spectrometry revealed large amounts of unidentified organic fluorine not captured by compound-specific analysis.

  • 16.
    Schultes, Lara
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Sandblom, Oskar
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Broeg, Katja
    Bignert, Anders
    Benskin, Jonathan
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Temporal trends (1981-2013) of per- and polyfluoroalkyl substances and unidentified organofluorine in Baltic codManuscript (preprint) (Other academic)
  • 17.
    Schultes, Lara
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    van Noordenburg, Carmen
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Spaan, Kyra
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Plassmann, Merle
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Roos, Anna
    Benskin, Jonathan
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    High Concentrations of Unidentified Extractable Organofluorine observed in Blubber from a Greenland Killer Whale (Orcinus orca)Manuscript (preprint) (Other academic)
  • 18.
    Schultes, Lara
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Vestergren, Robin
    Volkova, Kristina
    Westberg, Emelie
    Jacobson, Therese
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Per- and polyfluoroalkyl substances and fluorine mass balance in cosmetic products from the Swedish market: implications for environmental emissions and human exposure2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 12, p. 1680-1690Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFASs) are a diverse class of >4700 chemicals used in commercial products and industrial processes. Concerns surrounding PFASs are principally due to their widespread occurrence in humans and the environment and links to adverse health effects. One of the lesser known uses for PFASs is in cosmetic products (CPs) which come into contact with the skin (e.g. hair products, powders, sunblocks, etc.). In the present work, thirty-one CPs from five product categories (cream, foundation, pencil, powder and shaving foam) were analyzed for 39 PFASs by liquid chromatography-tandem mass spectrometry, as well as extractable organic fluorine (EOF) and total fluorine (TF) by combustion ion chromatography (CIC). This multi-platform approach enabled determination of the fraction of fluorine accounted for by known PFASs (i.e. fluorine mass balance). Foundations and powders contained 25 different PFASs with the most frequently detected being perfluorinated carboxylic acids (perfluoroheptanoic acid and perfluorohexanoic acid) and polyfluoroalkyl phosphate esters (PAPs). sigma(14)PAP concentrations up to 470 g g(-1) were measured in products listing mixtures of PAPs as an ingredient. For all samples, sigma(39)PFAS concentrations only explained a small fraction of the EOF and TF, pointing to the presence of unknown organic and/or inorganic fluorinated substances, including polymers. While creams, pencil and shaving foams did not contain measurable concentrations of any of the 39 PFASs targeted here, CIC revealed high to moderate TF content. Overall, these data highlight the need for further investigations into the occurrence of PFASs in CPs and their importance with regards to human and environmental exposure.

  • 19. Sedlak, Margaret D.
    et al.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Wong, Adam
    Grace, Richard
    Greig, Denise J.
    Per-and polyfluoroalkyl substances (PFASs) in San Francisco Bay wildlife: Temporal trends, exposure pathways, and notable presence of precursor compounds2017In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 185, p. 1217-1226Article in journal (Refereed)
    Abstract [en]

    Concentrations of perfluorooctane sulfonate (PFOS) in San Francisco Bay (SF Bay) wildlife have historically been among the highest reported globally. To track continuing exposures to PFASs and assess the impact of the 2002 phase-out of production of PFOS and related chemicals in the US, nine perfluoroalkyl carboxylic acids (PFCAs; C4-C12), three perfluoroalkyl sulfonic acids (PFSAs; C4, C6, C8) and perfluorooctane sulfonamide (PFOSA, a PFOS precursor) were measured in SF Bay cormorant eggs in 2012 and harbor seal serum sampled between 2009 and 2014. PFOS remained the dominant perfluoroalkyl acid (PFAA) in both cormorant eggs (36.1-466 ng/g) and seals (12.6-796 ng/g) from 2012 and 2014, respectively. Concentrations in seal and bird eggs from the South Bay have declined approximately 70% in both matrices. To elucidate potential pathways of exposure, prey fish, sediments and wastewater effluent were analyzed for PFASs, and in the case of sediment and effluent, a suite of PFAA precursors. PFOS was the dominant PFAA in prey fish and sediment. In effluent,, different mixtures of PFAAs were measured, with PFOS, PFHxA, and PFOA detected in the highest concentrations. Polyfluoroalkyl phosphate diesters (PFCA-precursors) were observed at concentrations over an order of magnitude higher than PFCAs in sediment, highlighting their importance as a potential, on-going source of PFCAs to SF Bay wildlife. These findings suggest that the PFOS phase-out has resulted in reduced burdens to wildlife in SF Bay, but that exposure to diverse and incompletely characterized PFASs continues.

  • 20.
    Su, Tong
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Tongji University, People's Republic of China .
    Deng, Huiping
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Radke, Michael
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Institute for Hygiene and Environment, Germany.
    Biodegradation of sulfamethoxazole photo-transformation products in a water/sediment test2016In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 148, p. 518-525Article in journal (Refereed)
    Abstract [en]

    Occurrence of the antibiotic sulfamethoxazole (SMX) in the aquatic environment is of concern due to its potential to induce antibiotic resistance in pathogenic bacteria. While degradation of SMX can occur by numerous processes, the environmental fate of its transformation products (TPs) remains poorly understood. In the present work, biodegradation of SMX photo-TPs was investigated in a water/sediment system. Photo-TPs were produced by exposing SMX to artificial sunlight for 48 h. The resulting mixture of 8 photo TPs was characterized using a combination of ultra-high performance liquid chromatography coupled to high-resolution mass spectrometry and tandem mass spectrometry, and then used in biodegradation experiments. Significant differences in transformation among SMX photo-TPs were observed in the water/sediment system, with four photo-TPs displaying evidence of biodegradation (dissipation half-lives [DT50] of 39.7 d for 3-amino-5-methylisoxazole, 12.7 d for 4-nitro-sulfamethxoazole, 7.6 d for an SMX isomer and 2.4 d for [C10H13N3O4S]), two displaying primarily abiotic degradation (DT50 of 31 d for sulfanilic acid and 74.9 d for 5-methylisoxazol-3-yl-sulfamate), and two photo TPs behaving largely recalcitrantly. Remarkably, TPs previously reported to be photo-stable also were persistent in biodegradation experiments. The most surprising observation was an increase in SMX concentrations when the irradiated solution was incubated, which we attribute to back-transformation of certain photo TPs by sediment bacteria (85% from 4-nitro-sulfamethoxazole). This process could contribute to exposure to SMX in the aquatic environment that is higher than one would expect based on the fate of SMX alone. The results highlight the importance of considering TPs along with their parent compounds when characterizing environmental risks of emerging contaminants.

  • 21.
    Yuan, Bo
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Chen, Chang-Er L.
    Bergman, Åke
    Determination of Chlorinated Paraffins by Bromide-Anion Attachment Atmospheric-Pressure Chemical Ionization Mass Spectrometry2018In: Environmental Science and Technology Letters, E-ISSN 2328-8930, Vol. 5, no 6, p. 348-353Article in journal (Refereed)
    Abstract [en]

    A novel method for the quantitative determination of chlorinated paraffins (CPs) was developed using bromide-anion attachment atmospheric-pressure chemical ionization mass spectrometry (APCI-MS). Bromoform was used to enhance ionization of CPs. Near exclusive formation of stable bromide adduct ions ([M + BR](-)) enabled accurate detection of individual CP congener groups (CnClm) with only a moderate-resolution quadrupole time-of-flight mass spectrometer. Furthermore, the method was free from interference commonly observed with chloride-anion attachment methods (e.g., decomposition ions [M + Cl - HCl](-)) that require deconvolution. Together with a CnClm-response-factor algorithm for quantifying short-chain CPs and a CnClm-pattern-reconstruction algorithm for quantifying medium- and long-chain CPs, method applicability was demonstrated on biota and sediment samples. These data were generated significantly faster and with improved selectivity and sensitivity versus those of conventional measurements by chloride-anion attachment APCI-MS.

  • 22.
    Zabaleta, Itsaso
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of the Basque Country (UPV/EHU), Spain.
    Bizkarguenaga, Ekhine
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of the Basque Country (UPV/EHU), Spain.
    Izagirre, Urtzi
    Negreira, Noelia
    Covaci, Adrian
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Prieto, Ailette
    Zuloaga, Olatz
    Biotransformation of 8: 2 polyfluoroalkyl phosphate diester in gilthead bream (Sparus aurata)2017In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 609, p. 1085-1092Article in journal (Refereed)
    Abstract [en]

    Polyfluoroalkyl phosphate esters (PAPs) are high production volume surfactants used in the food contact paper and packaging industry. PAPs may transform to persistent perfluoroalkyl carboxylic acids (PFCAs) under biotic conditions, but little is known about their fate and behavior in aquatic organisms. Here we report for the first time on the uptake, tissue distribution, and biotransformation of 8:2 polyfluoroalkyl phosphate diester (8:2 diPAP) in fish. Gilt-head bream (Sparus aurata) were dosed via the diet (8:2 diPAP at 29 mu g/g) for 7 days, during which time 8:2 diPAP and its transformation products were monitored in plasma, liver, muscle, gills, bile and brain. 8:2 diPAP tended to accumulate in liver, plasma and gills, and to a lesser extent in muscle, bile and brain. Several transformation products (observed previously in other organisms) were also observed inmost tissues and biofluids, including both saturated and unsaturated fluorotelomer acids (8:2 FTCA, 8:2 FTUCA, 7:3 FTCA), and perfluorooctanoic acid (PFOA). 8:2 FTCA was the major metabolite in all tissues/biofluids, except for bile, where PFOA occurred at the highest concentrations. Unexpectedly high PFOA levels (up to 3.7 ng/g) were also detected in brain. Phase 2 metabolites, which have been reported in fish following exposure to fluorotelomer alcohols, were not observed in these experiments, probably due to their low abundance. Nevertheless, the detection of PFOA indicates that exposure to PAPs may be an indirect route of exposure to PFCAs in fish.

  • 23.
    Zabaleta, Itsaso
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of the Basque Country (UPV/EHU), Spain.
    Bizkarguenaga, Ekhine
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of the Basque Country (UPV/EHU), Spain.
    Nunoo, Deborah B. O.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Schultes, Lara
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Leonel, Juliana
    Prieto, Ailette
    Zuloaga, Olatz
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Biodegradation and Uptake of the Pesticide Sulfluramid in a Soil-Carrot Mesocosm2018In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 52, no 5, p. 2603-2611Article in journal (Refereed)
    Abstract [en]

    N-ethyl perfluorooctane sulfonamide (EtFOSA) is the active ingredient of Sulfluramid, a pesticide which is used extensively in South America for control of leaf-cutting ants. Despite being a known precursor to perfluorooctanesulfonate (PFOS), the importance of EtFOSA as a source of environmental PFOS remains unclear. In the present work, uptake, leaching, and biodegradation of EtFOSA and its transformation products were assessed over 81 days in soil-carrot (Daucus carota ssp sativus) mesocosms for the first time. Experiments performed in the presence of carrot produced PFOS yields of up to 34% using a technical EtFOSA standard and up to 277% using Grao Forte, a commercial Sulfluramid bait formulation containing 0.0024% EtFOSA. Perfluorooctane sulfonamido acetate (FOSAA), perfluorooctane sulfonamide (FOSA), and perfluorooctanoic acid (PFOA) also formed over the course of the experiments, with the latter substance attributed to the presence of perfluorooctanamide impurities. The leachate contained low levels of transformation products and a high FOSA:PFOS ratio, consistent with recent observations in Brazilian surface water. In carrots, the more hydrophilic transformation products (e.g., PFOS) occurred primarily in the leaves, while the more hydrophobic products (e.g., FOSA, FOSAA, and EtFOSA) occurred in the peel and core. Remarkably, isomer-specific analysis revealed that the linear EtFOSA isomer biodegraded significantly faster than branched isomers. These data collectively show that the application of Sulfluramid baits can lead to the occurrence of PFOS in crops and in the surrounding environment, in considerably higher yields than previously thought.

  • 24.
    Ziarrusta, Haizea
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of the Basque Country (UPV/EHU), Spain.
    Mijangos, Leire
    Izagirre, Urtzi
    Plassmann, Merle M.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Anakabe, Eneritz
    Olivares, Maitane
    Zuloaga, Olatz
    Bioconcentration and Biotransformation of Amitriptyline in Gilt-Head Bream2017In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 51, no 4, p. 2464-2471Article in journal (Refereed)
    Abstract [en]

    Extensive global use of the serotonin norepinephrine reuptake inhibitor Amitriptyline (AMI) for treatment of mental health problems has led to its common occurrence in the aquatic environment. To assess AMI bioconcentration factors, tissue distribution, and metabolite formation in fish, we exposed gilt-head bream (Sparus aurata) to AMI in seawater for 7 days at two concentrations (0.2 mu g/L and 10 mu g/L). Day 7 proportional bioconcentration factors (BCFs) ranged from 6 (10 mu g/L dose, muscle) to 127 (0.2 mu g/L dose, brain) and were consistently larger at the low dose level. The relative tissue distribution of AMI was consistent at both doses, with concentrations decreasing in the order brain approximate to gill > liver > plasma > bile >> muscle. Using a suspect screening workflow based on liquid chromatography-high resolution (Orbitrap) mass spectrometry we identified 33 AMI metabolites (both Phase I and Phase II), occurring mostly in bile, liver and plasma. Ten structures are reported for the first time. Remarkably, all 33 metabolites retained the tricyclic ring structure common to tricyclic antidepressants, which may be toxicologically relevant. Collectively these data indicate that, in addition to AMI, a broad suite of metabolites should be included in biomonitoring campaigns in order to fully characterize exposure in aquatic wildlife.

  • 25.
    Ziarrusta, Haizea
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of the Basque Country (UPV/EHU), Spain.
    Ribbenstedt, Anton
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Mijangos, Leire
    Picart-Armada, Sergio
    Perera-Lluna, Alex
    Prieto, Ailette
    Izagirre, Urtzi
    Benskin, Jonathan P.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Olivares, Maitane
    Zuloaga, Olatz
    Etxebarria, Nestor
    Amitriptyline at an Environmentally Relevant Concentration Alters the Profile of Metabolites Beyond Monoamines in Gilt-Head Bream2019In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 38, no 5, p. 965-977Article in journal (Refereed)
    Abstract [en]

    The antidepressant amitriptyline is a widely used selective serotonin reuptake inhibitor that is found in the aquatic environment. The present study investigates alterations in the brain and the liver metabolome of gilt-head bream (Sparus aurata) after exposure at an environmentally relevant concentration (0.2 mu g/L) of amitriptyline for 7 d. Analysis of variance-simultaneous component analysis is used to identify metabolites that distinguish exposed from control animals. Overall, alterations in lipid metabolism suggest the occurrence of oxidative stress in both the brain and the liver-a common adverse effect of xenobiotics. However, alterations in the amino acid arginine are also observed. These are likely related to the nitric oxide system that is known to be associated with the mechanism of action of antidepressants. In addition, changes in asparagine and methionine levels in the brain and pantothenate, uric acid, and formylisoglutamine/N-formimino-L-glutamate levels in the liver could indicate variation of amino acid metabolism in both tissues; and the perturbation of glutamate in the liver implies that the energy metabolism is also affected. These results reveal that environmentally relevant concentrations of amitriptyline perturb a fraction of the metabolome that is not typically associated with antidepressant exposure in fish.

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