Person: Koschorreck, Jan
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Veröffentlichung Retrospective analysis of cyclic volatile methylsiloxanes in archived German fish samples covering a period of two decades(2020) Radermacher, Georg; Böhnhardt, Anna; Rüdel, Heinz; Koschorreck, Jan; Wesch, CharlotteCyclic volatile methylsiloxanes (cVMS) are widely applied chemicals used as intermediates in the production of silicon polymers or as ingredients in personal care products. cVMS are under scrutiny due to their environmental properties and their potential for long-range atmospheric transport, persistence and food web magnification. In 2018, the cVMS octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6) were identified as Substances of Very High Concern (SVHC) under the European REACH regulation. To obtain current data on the presence of cVMS in German waters, the spatial and temporal occurrence of D4, D5 and D6 in fillets of bream from major rivers archived in the German Environmental Specimen Bank (ESB) was analyzed with a GC-ICP-MS/MS coupling method. The spatial comparison of 17 sites for the year 2017 revealed that highest cVMS burdens occurred in samples from the Saar river (near to the French/German border). cVMS levels in fish from a lake in northern Germany did not exceed the limits of detection. For selected sites, time series covering the period from 1995 to 2017 were investigated. In most years D5 concentrations in fish were clearly higher than the observed D4 and D6 concentrations. Overall maximum D4 and D5 concentrations (about 320 and 7600 ng gâ Ì1 wet weight, respectively) were found at one Saar site in 2009. In three of five analyzed time series D5 concentrations peaked 2007â€Ì2011. In recent years, cVMS levels in fish decreased at almost all sites. To allow an assessment of the relevance of the detected cVMS fish concentrations these were compared to environmental quality standards (EQS) for D4 and D5 which were recently enacted in the context of the Swedish implementation of the European Water Framework Directive (WFD). The D5 EQS in fish was exceeded at four sites in several years in the investigated period and in the Saar even till 2017.Veröffentlichung Exploring unknown per- and polyfluoroalkyl substances in the German environment - The total oxidizable precursor assay as helpful tool in research and regulation(2021) Göckener, Bernd; Fettig, Ina; Fliedner, Annette; Rüdel, Heinz; Koschorreck, JanLimnetic, marine and soil samples of the German environmental specimen bank (ESB) were analyzed for per- and polyfluoroalkyl substances (PFAS) using target analysis and a modified total oxidizable precursor (TOP) assay (direct TOP assay (dTOP)) that works without prior extraction. Target analysis determined (Sigma)PFAS concentrations in bream livers of 8.7-282 (my)g kg-1 wet weight (ww) in 2019, with highest contaminations in the Rhine and lower Elbe. In bream fillet, concentrations were lower (<0.5-10.6 (my)g kg-1 (Sigma)PFAS). Contamination of suspended particulate matter (SPM) was highest in the upper Elbe downstream the Czech border (5.5 (my)g kg-1 dry weight (dw) in 2018). Herring gull eggs from the North and Baltic Seas showed (Sigma)PFAS levels around 53.0-69.6 (my)g kg-1 ww in 2019. In soil, concentrations ranged between <0.5 and 4.6 (my)g kg-1 dw with highest levels in the Dueben Heath near Leipzig and the low mountain range Solling. PFOS dominated in most samples. Of the targeted precursors, only FOSA, EtFOSAA, MeFOSAA, 6:2-FtS and 6:2 diPAP were found. Replacement chemicals (ADONA, HFPO-DA, F-53B) were not detected. The dTOP assay revealed that considerable amounts of precursors were present at most riverine sampling sites. Particularly high precursor concentrations were observed in samples from the Upper Elbe at the Czech border and the Upper and Middle Rhine. In herring gull eggs and most soil samples, though, concentrations of precursors were low. Time trend analysis showed decreasing trends for most detected PFAS since 2005. In SPM, however, C4-C6 perfluoroalkyl carboxylic acids seem to increase indicating growing use of precursors based on shorter fluorinated chains. The results demonstrate that target analysis detects only a minor fraction of the PFAS burdens in environmental samples. The dTOP assay can support risk assessment and chemical monitoring with more comprehensive exposure data of the actual contamination. © 2021 The Author(s).Veröffentlichung Making use of apex predator sample collections: an integrated workflow for quality assured sample processing, analysis and digital sample freezing of archived samples(2022) Badry, Alexander; Rüdel, Heinz; Göckener, Bernd; Koschorreck, Jan; Treu, GabrieleUsing monitoring data from apex predators for chemicals risk assessment can provide important information on bioaccumulating as well as biomagnifying chemicals in food webs. A survey among European institutions involved in chemical risk assessment on their experiences with apex predator data in chemical risk assessment revealed great interest in using such data. However, the respondents indicated that constraints were related to expected high costs, lack of standardisation and harmonised quality criteria for exposure assessment, data access, and regulatory acceptance/application. During the Life APEX project, we demonstrated that European sample collections (i.e. environmental specimen banks (ESBs), research collection (RCs), natural history museums (NHMs)) archive a large variety of biological samples that can be readily used for chemical analysis once appropriate quality assurance/control (QA/QC) measures have been developed and implemented. We therefore issued a second survey on sampling, processing and archiving procedures in European sample collections to derive key quality QA/QC criteria for chemical analysis. The survey revealed great differences in QA/QC measures between ESBs, NHMs and RCs. Whereas basic information such as sampling location, date and biometric data were mostly available across institutions, protocols to accompany the sampling strategy with respect to chemical analysis were only available for ESBs. For RCs, the applied QA/QC measures vary with the respective research question, whereas NHMs are generally less aware of e.g. chemical cross-contamination issues. Based on the survey we derived key indicators for assessing the quality of biota samples that can be easily implemented in online databases. Furthermore, we provide a QA/QC workflow not only for sampling and processing but also for the chemical analysis of biota samples. We focussed on comprehensive analytical techniques such as non-target screening and provided insights into subsequent storage of high-resolution chromatograms in online databases (i.e. digital sample freezing platform) to ultimately support chemicals risk assessment. © 2022 The Authors.Veröffentlichung Selection and application of trophic magnification factors for priority substances to normalize freshwater fish monitoring data under the European Water Framework Directive: a case study(2020) Rüdel, Heinz; Duffek, Anja; Kosfeld, Verena; Fliedner, Annette; Koschorreck, Jan; Rauert, CarenBackground The European Water Framework Directive (WFD) requires the monitoring of biota-preferably fish - to check the compliance of tissue concentrations of priority substances (PS) against substance-specific environmental quality standards (EQSs). In monitoring programs, different fish species are covered, which often are secondary consumers with a trophic level (TL) of about 3. For harmonization, a normalization of monitoring data to a common trophic level is proposed, i.e., TL 4 (predatory fish) in freshwaters, so that data would be sufficiently protective. For normalization, the biomagnification properties of the chemicals can be considered by applying substance-specific trophic magnification factors (TMFs). Alternatively, TL-corrected biomagnification factors (BMFTLs) may be applied. Since it is impractical to derive site-specific TMFs or BMFTLs, often data from literature will be used for normalization. However, available literature values for TMFs and BMFTLs are quite varying. In the present study, the use of literature-derived TMFs and BMFTLs in data normalization is studied more closely. Results An extensive literature evaluation was conducted to identify appropriate TMFs for the WFD PS polybrominated diphenyl ethers (PBDE), hexachlorobenzene, perfluorooctane sulfonate (PFOS), dioxins and dioxin-like compounds (PCDD/F+dl-PCB), hexabromocyclododecane, and mercury. The TMFs eventually derived were applied to PS monitoring data sets of fish from different trophic levels (chub, bream, roach, and perch) from two German rivers. For comparison, PFOS and PBDE data were also normalized using literature-retrieved BMFTLs. Conclusions The evaluation illustrates that published TMFs and BMFTLs for WFD PS are quite variable and the selection of appropriate values for TL 4 normalization can be challenging. The normalized concentrations partly included large uncertainties when considering the range of selected TMFs, but indicated whether an EQS exceedance at TL 4 can be expected. Normalization of the fish monitoring data revealed that levels of substances accumulating in the food web (TMF or BMF>1) can be underestimated when relying on fish with TL<4 for EQS compliance assessment. The evaluation also revealed that TMF specifically derived for freshwater ecosystems in Europe would be advantageous. Field-derived BMFTLs seemed to be no appropriate alternative to TMFs, because they can vary even stronger than TMFs. © The Author(s) 2020Veröffentlichung Tissue concentrations of per- and polyfluoroalkyl substances (PFAS) in German freshwater fish: derivation of fillet-to-whole fish conversion factors and assessment of potential risks(2022) Rüdel, Heinz; Duffek, Anja; Radermacher, Georg; Fliedner, Annette; Koschorreck, JanThe European Water Framework Directive requires monitoring of bioaccumulative contaminants in fish to assess risks to human health by fish consumption and wildlife by secondary poisoning of predators. The list of priority substances for which environmental quality standards (EQSs) have been derived covers also perfluorooctane sulfonic acid (PFOS). No EQSs have yet been set for other per- and polyfluoroalkyl substances (PFAS) that are frequently detected in fish and of which some have a non-negligible risk potential compared to PFOS. As a case study, burdens for a set of PFAS were investigated for different fish species from five German freshwater sites and a Baltic Sea lagoon. PFAS concentrations were determined for composite samples of both, fillet and whole fish. On average, sum concentrations of C9-C14 perfluoroalkyl carboxylic acids, which will be banned in the European Union in 2023, reached 87% and 82% of the PFOS burdens in fillet and whole fish, respectively. The potential risk of several PFAS other than PFOS was assessed using a previously suggested relative potency factor approach, which is also applied for a proposed EQS revision. Only five of 36 fillet samples (mostly perch) exceeded the current EQS for PFOS alone. By contrast, all fillet samples exceeded the newly proposed draft EQS, which considers potential effects of further PFAS but also a lower tolerable intake value. Additionally, the dataset was used to derive fillet-to-whole fish conversion factors, which can be applied to assess human health risks by consumption of fillet if only whole fish concentrations are available. © 2021 The AuthorsVeröffentlichung Per- and polyfluoroalkyl substances in the German environment - Levels and patterns in different matrices(2020) Kotthoff, Matthias; Biegel-Engler, Annegret; Fliedner, Annette; Rüdel, Heinz; Koschorreck, JanPer- and polyfluoroalkyl substances (PFAS) in the environment mostly originate from emissions of previously unregulated PFAS. However, there are also many documented incidents of accidental releases. To track such releases, it is essential to distinguish between typical background contamination and legally relevant incidents. This requires a comprehensive overview of all PFAS present in the environment, which is currently only possible to a limited extent due to the large variety of individual compounds. In the present study, a multimethod for capturing 41 PFAS including perfluoroalkyl acid (PFAA) precursors is introduced. The applicability of the method was tested on terrestrial, freshwater and marine samples from the German Environmental Specimen Bank (ESB), thereby providing a rough overview of PFAS contamination in German environment. Special focus was put on soil samples from ESB sites across Germany in comparison to soil samples from a polluted site in south-west Germany. The method was successfully applied to environmental samples. In total, 31 PFAS were detected, among them PFAA precursors and fluorinated ethers. Substance patterns differed between sites and matrices. In ESB soil samples from 2014 (n = 11), the sum of all captured PFAS ranged between 0.75 and 19.5 (my)g kg-1 dry weight (dw), while concentrations between 416 (my)g kg-1 and 3530 (my)g kg-1 were detected in samples from the incident site (n = 10). In other matrices, total PFAS concentrations were magnitudes lower. Highest concentrations were observed for PFOS in bream livers from the Saale (226 (my)g kg-1). Given the heterogeneous patterns, it will require further broadly-based monitoring data to allow for a solid estimation of relevant background levels. The data provided here may support the differentiation between background levels and hotspot contaminations. ©2020 The AuthorsVeröffentlichung Environmental specimen banks and the European Green Deal(2022) Fliedner, Annette; Rüdel, Heinz; Göckener, Bernd; Koschorreck, JanThe study highlights the potential of Environmental Specimen Banks (ESBs) for implementing the Zero Pollution Ambition and the Biodiversity Strategy of the European Green Deal. By drawing on recent monitoring studies of European ESBs, we illustrate the role ESBs already play in assessing the state of ecosystems in Europe and how they help to make developments over time visible. The studies reveal the ubiquitous presence of per- and polyfluoroalkyl substances, halogenated flame retardants, chlorinated paraffins, plasticizers, cyclic volatile methyl siloxanes, UV-filters, pharmaceuticals, and microplastics in the European environment. Temporal trends demonstrate the effectiveness of European regulations on perfluorooctane sulfonic acid, pentabrominated diphenylethers and diethylhexyl phthalate, but also point to the rise of substitutes such as non-phthalate plasticizers and short-chain perfluoroalkyl substances. Other studies are wake-up calls indicating the emergence of currently unregulated compounds such as long-chain chlorinated paraffins. Ecological studies show temporal trends in biometric parameters and stable isotope signatures that suggest long-term changes in environmental conditions. Studies on biodiversity of ecosystems using environmental DNA are still in their beginnings, but here too there is evidence of shifts in community composition that can be linked to changing environmental conditions. This review demonstrates the value of ESBs (a) for describing the status of the environment, (b) for monitoring temporal changes in environmental pollution and the ecologic condition of ecosystems and thereby (c) for supporting regulators in prioritizing their actions towards the objectives of the Green Deal. © 2022 ElsevierVeröffentlichung Food web on ice: a pragmatic approach to investigate the trophic magnification of chemicals of concern(2021) Kosfeld, Verena; Koschorreck, Jan; Rüdel, Heinz; Schlechtriem, Christian; Rauert, CarenBackground The trophic magnification factor (TMF) is a metric that describes the average trophic magnification of a chemical through a food web. TMFs may be used for the risk assessment of chemicals, although TMFs for single compounds can vary considerably between studies despite thorough guidance available in the literature to eliminate potential sources of error. The practical realization of a TMF investigation is quite complex and often only a few chemicals can be investigated due to low sample masses. This study evaluated whether a pragmatic approach involving the large-scale cryogenic sample preparation practices of the German Environmental Specimen Bank (ESB) is feasible. This approach could provide sufficient sample masses for a reduced set of samples allowing screenings for a broad spectrum of substances and by that enabling a systematic comparison of derived TMFs. Furthermore, it was assessed whether plausible TMFs can be derived with the â€ÌFood web on iceâ€Ì approach via a comparison with literature TMF values. Results This investigation at Lake Templin near Potsdam is the first TMF study for a German freshwater ecosystem and aimed to derive TMFs that are appropriate for regulatory purposes. A set of 15 composite biota samples was obtained and analyzed for an extended set of benchmark chemicals such as persistent organic pollutants, mercury and perfluoroalkyl substances. TMFs were calculated for all substances that were present in†>†80% of the biota samples. For example, in the case of polychlorinated biphenyls, TMFs from 1.7 to 2.5 were determined and comparisons to literature TMFs determined in other freshwater ecosystems showed similarities. We showed that 32 out of 35 compounds analyzed had TMFs significantly above 1. In the remaining three cases, the correlations were not statistically significant. Conclusions The derived food web samples allow for an on-demand analysis and are ready-to-use for additional investigations. Since substances with non-lipophilic accumulation properties were also included in the list of analyzed substances, we conclude that the 'Food web on ice' provides samples which could be used to characterize the trophic magnification potential of substances with unknown bioaccumulation properties in the future which in return could be compared directly to the benchmarking patterns provided here. © The Author(s) 2021Veröffentlichung Chemicals of emerging concern in marine specimens of the German Environmental Specimen Bank(2020) Fliedner, Annette; Rüdel, Heinz; Dreyer, Annekatrin; Koschorreck, JanBackground Descriptor 8 of the Marine Strategy Framework Directive (MSFD) (Directive 2008/56/EC) addresses the good environmental status with regard to pollution of marine waters by chemical contaminants. Commission decision (EU) 2017/848 lays down the criteria and methodological standards on good environmental status of marine waters. Member States, in regional or subregional cooperation, shall establish lists of relevant contaminants beside those already covered by the Water Framework Directive (WFD). To provide information on emerging contaminants in marine biota, the German Environmental Specimen Bank (ESB) has compiled data of blue mussels and eelpouts from coastal sites in the North and Baltic Seas. Substances identified by the International Council for the Exploration of the Sea (ICES) as of emerging concern for the marine environment have been used as a starting point. Results and conclusions The study presents data of 19 emerging flame retardants and degradation products, 40 per- and polyfluoroalkyl substances (PFAS) and three cyclic volatile methylsiloxanes (cVMS). Among the emerging flame retardants, only Dec 602 was detected in all samples of 2015. Dec 604, Cl10-antiDP, 1,5-DPMA, EH-TBB, PBEB, TBP-AE, BATE, BTBPE and HBBz were constantly <†limit of quantification (LOQ). Time trends were barely detected. Legacy PBDE still dominates in most samples. PFAS concentrations were usually higher in samples from the North Sea sites compared to samples from the Baltic Sea. PFOS dominated in most samples. Increasing trends over time were detected for PFNA, PFDA and PFDoDA at the Baltic Sea site and for PFDA at one North Sea site. Concentrations of the cVMS D4, D5 and D6 were below the detection limit at the ESB sampling sites. Based on the results, it should be considered to include the emerging flame retardants DP and Dec 602 and the long-chain perfluoroalkyl substances PFNA, PFDA, PFUnDA and PFDoDA in a regular monitoring in the North and Baltic Seas. © The Author(s) 2020Veröffentlichung Long-term trends of Per- and Polyfluoroalkyl Substances (PFAS) in suspended particular matter from German rivers using the direct Total Oxidizable Precursor (dTOP) assay(2022) Göckener, Bernd; Badry, Alexander; Fliedner, Annette; Rüdel, Heinz; Koschorreck, JanSuspended particulate matter (SPM) from 13 riverine sampling sites of the German Environmental Specimen Bank collected between 2005 and 2019 was retrospectively investigated for per- and polyfluoroalkyl substances (PFAS). The samples were analyzed both by target analysis for 41 PFAS and by a modified total oxidizable precursor (dTOP) assay to capture also unknown precursors. Temporal trends and spatial differences were investigated by generalized linear modeling (GLM). Time trend analysis across all rivers showed decreasing trends for (Sigma)PFCA and (Sigma)PFSA concentrations in SPM. Trends based on target analysis ((Sigma)PFCAtarget: -10.0%, (Sigma)PFSAtarget: -8.2%) were more pronounced than in the dTOP analysis ((Sigma)PFCAdTOP: -4.2%; (Sigma)PFSAdTOP: -5.3%), suggesting that conventional target analysis overestimated actual decreases as precursors are not considered. (Sigma)PFAS concentrations determined by dTOP assay were 1.3-145 times higher as compared to target analysis, indicating substantial amounts of unknown precursors in the samples. The (Sigma)PFASdTOP/(Sigma)PFAStarget ratio increased at all sites between 2005 and 2019. Contamination was highest in SPM from the Elbe tributary Mulde downstream of a large industrial park. The results underscore the need to go beyond conventional target analysis and include precursors when assessing PFAS contamination in the environment. The dTOP assay is a suitable tool for this purpose. © 2022, American Chemical Society