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Exposure to flame retardants in European children - results from the HBM4EU aligned studies

Many legacy and emerging flame retardants (FRs) have adverse human and environmental health effects. This study reports legacy and emerging FRs in children from nine European countries from the HBM4EU aligned studies. Studies from Belgium, Czech Republic, Germany, Denmark, France, Greece, Slovenia, Slovakia, and Norway conducted between 2014 and 2021 provided data on FRs in blood and urine from 2136 children. All samples were collected and analyzed in alignment with the HBM4EU protocols. Ten halogenated FRs were quantified in blood, and four organophosphate flame retardants (OPFR) metabolites quantified in urine. Hexabromocyclododecane (HBCDD) and decabromodiphenyl ethane (DBDPE) were infrequently detected (<16% of samples). BDE-47 was quantified in blood from Greece, France, and Norway, with France (0.36 ng/g lipid) having the highest concentrations. BDE-153 and -209 were detected in <40% of samples. Dechlorane Plus (DP) was quantified in blood from four countries, with notably high median concentrations of 16 ng/g lipid in Slovenian children. OPFR metabolites had a higher detection frequency than other halogenated FRs. Diphenyl phosphate (DPHP) was quantified in 99% of samples across 8 countries at levels ~5 times higher than other OPFR metabolites (highest median in Slovenia of 2.43 ng/g lipid). FR concentrations were associated with lifestyle factors such as cleaning frequency, employment status of the father of the household, and renovation status of the house, among others. The concentrations of BDE-47 in children from this study were similar to or lower than FRs found in adult matrices in previous studies, suggesting lower recent exposure and effectiveness of PBDE restrictions. © 2022 The Authors

FT-ICR-MS Data Used to Trace Variations of Organic Carbon Sourcing Along a Trans-Himalayan River, Central Nepal

Abstract

Equilibrium sampling of suspended particulate matter as a universal proxy for fish and mussel monitoring

Wernicke, Theo; Abel, Sebastian; Escher, Beate I.; Koschorreck, Jan; Rüdel, Heinz; Jahnke, Annika Ecotoxicol Environ Saf 232 (2022), 113285, online 8. Februar 2022 Bioaccumulation of persistent and hydrophobic organic compounds in the aquatic environment puts secondary consumers, such as fish, at risk. To assess their exposure, monitoring programs with high numbers of individuals have been conducted worldwide over decades that require major efforts and raise ethical issues. This study aimed at testing suspended particulate matter (SPM) as an alternative and accessible abiotic matrix to estimate the internal exposure concentrations of such chemicals in fish and mussels. Muscle tissues of bream (Abramis brama), tissues of zebra mussels (Dreissena polymorpha) and SPM were collected from four major German rivers, Elbe, Danube, Saar and Saale, in 2018 within the national monitoring program of the German Environmental Specimen Bank. We used (i) total solvent extraction for biota samples to quantify the lipid-normalized concentrations of polychlorinated biphenyls, polycyclic aromatic hydrocarbons and hexachlorobenzene and (ii) passive equilibrium sampling of SPM to derive equilibrium partitioning concentrations in lipids and (iii) set these independent data sets into context. Since the ratio of lipid-normalized concentration / equilibrium partitioning concentration in lipids was in most cases < 1.0, SPM may serve as a conservative proxy for the internal concentration of bream and mussels, although bream of high age (i.e., older than 10 years) showed a tendency for this ratio to exceed 1.0. This observation indicates that age-dependent biomagnification can exceed the predictions based on thermodynamic equilibrium relative to SPM. doi: 10.1016/j.ecoenv.2022.113285

Screening the baseline fish bioconcentration factor of various types of surfactants using phospholipid binding data

Fish bioconcentration factors (BCFs) are commonly used in chemical hazard and risk assessment. For neutral organic chemicals BCFs are positively correlated with the octanol-water partition ratio (KOW), but KOW is not a reliable parameter for surfactants. Membrane lipid-water distribution ratios (DMLW) can be accurately measured for all kinds of surfactants, using phospholipid-based sorbents. This study first demonstrates that DMLW values for ionic surfactants are more than 100â€č000 times higher than the partition ratio to fish-oil, representing neutral storage lipid. A non-ionic alcohol ethoxylate surfactant showed almost equal affinity for both lipid types. Accordingly, a baseline screening BCF value for surfactants (BCFbaseline) can be approximated for ionic surfactants by multiplying DMLW by the phospholipid fraction in tissue, and for non-ionic surfactants by multiplying DMLW by the total lipid fraction. We measured DMLW values for surfactant structures, including linear and branched alkylbenzenesulfonates, an alkylsulfoacetate and an alkylethersulfate, bis(2-ethylhexyl)-surfactants (e.g., docusate), zwitterionic alkylbetaines and alkylamine-oxides, and a polyprotic diamine. Together with sixty previously published DMLW values for surfactants, structure-activity relationships were derived to elucidate the influence of surfactant specific molecular features on DMLW. For 23 surfactant types, we established the alkyl chain length at which BCFbaseline would exceed the EU REACH bioaccumulation (B) threshold of 2000 L kg-1, and would therefore require higher tier assessments to further refine the BCF estimate. Finally, the derived BCFbaseline are compared with measured literature in vivo BCF data where available, suggesting that refinements, most notably reliable estimates of biotransformation rates, are needed for most surfactant types. © Royal Society of Chemistry 2021

Time trend of exposure to dechloranes: Plasma samples of German young adults from the environmental specimen bank collected from 1995 to 2017

Fromme, Hermann; Thomsen, Cathrine; Aschenbrenner, Bettina; Haug, Line Småstuen; Weber, Till; Kolossa-Gehring, Marike; Völkel, Wolfgang; Schober, Wolfgang International Journal of Hygiene and Environmental Health 229 (2020), August 2020, 113593; online 12. August 2020 Dechloranes, like Dechlorane Plus ® are commonly used flame retardants identified by the EU as substances of very high concern (SVHC) because of their persistence and bioaccumulation potential. To characterize the dechlorane exposure of Germans in the last two decades, 180 archived blood plasma samples of the German Environmental Specimen Bank (students aged 20–29 years) collected at six time points between 1995 and 2017 were analyzed for four dechloranes; namely Dechlorane Plus ® (syn- and anti-DDC-CO), dechlorane 602 (DDC-DBF), and dechlorane 603 (DDC-Ant). These were quantified using a GC-MS/MS method. Overall, anti- and syn-DDC-CO were detected in 88% and 98% of the samples, whereas DDC-DBF and DDC-Ant were found in 40% and 37% of the samples, respectively. The median (95th percentile) values were 1.0 ng/g lipid weight (l.w.) (3.0 ng/g l.w.). for anti-DDC-CO, 0.6 ng/g l.w (1.9 ng/g l.w.). for syn–DDC-CO, 0.1 ng/g l.w (0.6 ng/g l.w.). for DDC-DBF, and 0.1 ng/g l.w (0.2 ng/g l.w.). for DDC-Ant. The 95th percentile concentrations of the sum of syn- and anti-DDC-CO decreased from 4.2 ng/g l.w. in 1995, to 2.9 ng/g l.w. in 1999, and subsequently increased to 3.7 ng/g l.w. in 2008, and up to 5.9 ng/g l.w. in 2017. A statistically significant decrease with time was observed for DDC-DBF and DDC-Ant, but not for DDC-CO. Our medians found in blood samples in 2017 are similar to those observed in Germany in 2013/14, but higher compared to values reported in other European countries. Overall, more toxicological and monitoring data is needed to better characterize the potential impact on health. doi: 10.1016/j.ijheh.2020.113593

Polystyrene microplastics do not affect juvenile brown trout (Salmo trutta f. fario) or modulate effects of the pesticide methiocarb

Background There has been a rising interest within the scientific community and the public about the environmental risk related to the abundance of microplastics in aquatic environments. Up to now, however, scientific knowledge in this context has been scarce and insufficient for a reliable risk assessment. To remedy this scarcity of data, we investigated possible adverse effects of polystyrene particles (104 particles/L) and the pesticide methiocarb (1 mg/L) in juvenile brown trout (Salmo trutta f. fario) both by themselves as well as in combination after a 96 h laboratory exposure. PS beads (density 1.05 g/mL) were cryogenically milled and fractionated resulting in irregular-shaped particles (<50 (micro)m). Besides body weight of the animals, biomarkers for proteotoxicity (stress protein family Hsp70), oxidative stress (superoxide dismutase, lipid peroxidation), and neurotoxicity (acetylcholinesterase, carboxylesterases) were analyzed. As an indicator of overall health, histopathological effects were studied in liver and gills of exposed fish. Results Polystyrene particles by themselves did not influence any of the investigated biomarkers. In contrast, the exposure to methiocarb led to a significant reduction of the activity of acetylcholinesterase and the two carboxylesterases. Moreover, the tissue integrity of liver and gills was impaired by the pesticide. Body weight, the oxidative stress and the stress protein levels were not influenced by methiocarb. Effects caused by co-exposure of polystyrene microplastics and methiocarb were the same as those caused by methiocarb alone. Conclusions Overall, methiocarb led to negative effects in juvenile brown trout. In contrast, polystyrene microplastics in the tested concentration did not affect the health of juvenile brown trout and did not modulate the toxicity of methiocarb in this fish species. © The Author(s) 2020

Biota monitoring under the Water Framework Directive: On tissue choice and fish species selection

Fliedner, Annette; Rüdel, Heinz; Lohmann, Nina; Buchmeier, Georgia; Koschorreck, Jan Environmental Pollution 235 (2018), 129-140; online 23. Dezember 2017 The study addresses the topic of suitable matrices for chemical analysis in fish monitoring and discusses the effects of data normalization in the context of the European Water Framework Directive (WFD). Differences between species are considered by comparing three frequently monitored species of different trophic levels, i.e., chub (Squalius cephalus, n = 28), (bream, Abramis brama, n = 11), and perch (Perca fluviatilis, n = 19) sampled in the German Danube. The WFD priority substances dioxins, furans and dioxin-like polychlorinated biphenyls (PCDD/F + dl-PCB), polybrominated diphenyl ethers (PBDE), α-hexabromocyclododecane (α-HBCDD), hexachlorobenzene (HCB), mercury (Hg), and perfluorooctane sulfonic acid (PFOS) as well as non-dioxin-like (ndl)-PCB were analyzed separately in fillet and carcass and whole body concentrations were calculated. Hg was analyzed in individual fish fillets and carcasses, all other substances were determined in pool samples, which were compiled on the basis of fish size (3 chub pools, 1 bream pool, 2 perch pools). The data were normalized to 5% lipid weight (or 26% dry mass in the case of Hg and PFOS) for comparison between matrices and species. Hg concentrations were generally higher in fillet than in whole fish (mean whole fish-to-fillet ratio: 0.7) whereas all other substances were mostly higher in whole fish. In the case of lipophilic substances these differences leveled after lipid normalization. Significant correlations (p ≤ .05) were detected between Hg and fish weight and age. Hg concentrations varied least among younger fish. PCDD/F, dl-PCB, ndl-PCB, PBDE, α-HBCDD and HCB correlated significantly (p ≤ .05) with lipid concentrations. Fillet-to-whole fish conversion equations and/or conversion factors were derived for all substances except α-HCBDD. Although more data also for individual fish would be desirable the results are nevertheless a step on the way to translate fillet concentrations of priority substances to whole fish concentrations. doi:10.1016/j.envpol.2017.12.052

Biota monitoring and the Water Framework Directive - can normalization overcome shortcomings in sampling strategies?

Fliedner, Annette; Rüdel, Heinz; Teubner, Diana; Buchmeier, Georgia; Lowis, Jaqueline; Heiss, Christiane; Wellmitz, Jörg; Koschorreck, Jan Environ Sci Pollut Res Int. (2016), online 18. August 2016 We compare the results of different monitoring programs regarding spatial and temporal trends of priority hazardous substances of the European Water Framework Directive (WFD). Fish monitoring data for hexachlorobenzene (HCB), mercury (Hg), and perfluorooctane sulfonic acid (PFOS) sampled in German freshwaters between the mid-1990s and 2014 were evaluated according to the recommendations of the 2014 adopted WFD guidance document on biota monitoring, i.e., normalization to 5 % lipid content (HCB) or 26 % dry mass (Hg, PFOS) and adjustment to trophic level (TL) 4. Data of the German Environmental Specimen Bank (ESB) (annual pooled samples of bream) were compared to monitoring data of the German federal states (FS), which refer to individual fish of different species. Significant decreasing trends (p < 0.01) were detected for Hg in bream (Abramis brama) sampled by both, the ESB and the FS between 1993 and 2013 but not for FS samples comprising different fish species. Data for HCB and PFOS were more heterogeneous due to a smaller database and gave no consistent results. Obviously, normalization could not compensate differences in sampling strategies. The results suggest that the data treatment procedure proposed in the guidance document has shortcomings and emphasize the importance of highly standardized sampling programs in trend monitoring or whenever results between sites have to be compared. doi:10.1007/s11356-016-7442-2

Biometric parameters of the bream (Abramis brama ) as indicators for long-term changes in fish health and environmental quality - data from the German ESB

Teubner, Diana; Paulus, Martin; Veith, Michael; Klein, Roland Environ Sci Pollut Res 22 (2015), 3, 1620-1627 Piscifaunal health depends upon the state and quality of the aquatic environment. Variations in physical condition of fish may therefore be attributed to changes in environmental quality. Based on time series of up to 20 years of biometric data of bream from multiple sampling sites of the German environmental specimen bank (ESB), this study assessed whether changes in biometric parameters are able to indicate long-term alterations in fish health and environmental quality. Evaluated biometric parameters of fish health comprised length and weight of individuals of a defined age class, the condition factor, lipid content and hepatosomatic index (HSI). Although there are negative trends of the HSI, the overall development of health parameters can be interpreted as positive. This seems to suggest that health parameters conclusively mirror the long-term improvement of water quality in the selected rivers. However, the applicability of the condition factor as well as lipid content as indicators for fish health remained subject to restrictions. Altogether, the results from the ESB confirmed the high value of biometric parameters for monitoring of long-term changes in state and quality of aquatic ecosystems. doi: 10.1007/s11356-014-3008-3

Retrospective study of triclosan and methyl-triclosan residues in fish and suspended particulate matter: Results from the German Environmental Specimen Bank

Rüdel, Heinz; Böhmer, Walter; Müller, Martin; Fliedner, Annette; Ricking, Mathias; Teubner, Diana; Schröter-Kermani, Christa Chemosphere 91 (2013), 11, 1517-1524 A retrospective monitoring of triclosan (TCS; period 1994-2003 and 2008) and its potential transformation product methyl-triclosan (MTCS; period 1994-2008) was performed using archived fish samples from German rivers (16 sites, including Elbe and Rhine). At four of these sites suspended particulate matter (SPM) was also investigated covering the period 2005-2007. Samples were analyzed by GC/MS, either directly (MTCS) or after derivatization (TCS). TCS burdens of fish muscle tissue ranged from <0.2-3.4 ng g -1 ww (wet weight; corresponding to <2-69 ng g -1 lw, lipid weight) without apparent concentration trends over time. MTCS was detected at considerably higher concentrations in fish ranging from 1.0-33 ng g -1 ww (47-1010 ng g -1 lw) and increased until about 2003-2005. Thereafter, concentrations generally were lower, although at some sites single higher values were observed in recent years. In SPM, decreasing MTCS concentrations in the range 1-4 ng g -1 dry weight were detected while TCS was always below the limit of quantification. Assuming that MTCS concentrations are correlated to TCS consumption, the observed decrease in MTCS levels may be partly a result of the voluntary renunciation of TCS use in detergents for, e.g., laundry or dishwashing declared by a manufacturers’ association in 2001. Because of a lack of ecotoxicity studies for MTCS, a QSAR-derived predicted no effect concentration (PNEC) was compared to averaged ambient water concentrations of fish which were calculated from maximum tissue residues by applying an appropriate bioconcentration factor from literature. Since these calculated water concentrations were below the PNEC it is assumed that MTCS alone poses no immediate risk to aquatic organism. The conversion to a PNEC for SPM organisms and comparison with detected SPM levels of MTCS also revealed no risk. doi:10.1016/j.chemosphere.2012.12.030

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