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Veröffentlichung Current levels and trends of selected EU Water Framework Directive priority substances in freshwater fish from the German environmental specimen bank(2016) Fliedner, Annette; Lohmann, Nina; Koschorreck, Jan; Rüdel, Heinz; Teubner, Diana; Wellmitz, JörgUnder the German environmental specimen bank programme bream (Abramis brama) were sampled in six German rivers and analysed for the priority hazardous substances dicofol, hexabromocyclododecane (HBCDD), hexachlorobenzene (HCB), hexachlorobutadiene (HCBD), heptachlor þ heptachlor epoxide (HC þ HCE), polybrominated diphenylethers (PBDEs), polychlorinated dibenzo-p-dioxins and -furans and dioxin-like polychlorinated biphenyls (PCDD/Fs þ dl-PCBs), and perfluorooctane sulfonic acid (PFOS). The aim was to assess compliance with the EU Water Framework Directive environmental quality standards for biota (EQSBiota) for the year 2013, and to analyse temporal trends for those substances that are of special concern. General compliance was observed for dicofol, HBCDD and HCBD whereas PBDEs exceeded the EQSBiota at all sites. For all other substances compliance in 2013 varied between locations. No assessment was possible for HC þ HCE at some sites where the analytical sensitivity was not sufficient to cover the EQSBiota. Trend analysis showed decreasing linear trends for HCB and PFOS at most sampling sites between 1995 and 2014 indicating that the emission reduction measures are effective. Mostly decreasing trends or constant levels were also observed for PCDD/Fs and dl-PCBs. In contrast, increasing trends were detected for PBDEs and HBCDD which were especially pronounced at one Saar site located downstream of the industries and conurbation of Saarbrücken and V€olklingen. This finding points to new sources of emissions which should be followed in the coming years. Quelle: www.sciencedirect.comVeröffentlichung Assessment of seafood contamination under the marine strategy framework directive: contributions of the German environmental specimen bank(2018) Fliedner, Annette; Rüdel, Heinz; Knopf, Burkhard; Koschorreck, JanDescriptor 9 (D9) of the European Union Marine Strategy Framework Directive refers to the compliance of contaminant levels in fish and other seafood of a defined marine region or subregion with human health threshold values. This requires georeferenced samples that are often difficult to obtain when relying on commercial fisheries or programs designed for monitoring human exposure. The present study examines whether georeferenced samples of blue mussel (Mytilus edulis) and eelpout (Zoarces viviparus) fillet of the German environmental specimen bank (ESB) can be used in this context. The suitability of the ESB samples, procedures, and analytical methods is evaluated with respect to D9 requirements. Based on ESB data for the D9 relevant contaminants Pb, Cd, Hg, â Ì4 PAHs, PCDD/Fs, dioxin-like (dl)-PCBs, and indicator non-dl-PCBs and the potentially relevant substances TBT, PFOS, PBDE, and HBCDD, the Good Environmental Status for D9 is assessed at the ESB sites in the North and Baltic Seas. The overall evaluation indicates that ESB samples are suitable for D9 assessment with the limitation that only coastal areas of the North and Baltic Seas are covered. Over a period of up to 30 years, concentrations of the D9 relevant contaminants were well below the maximum levels allowed for human consumption. © The Author(s) 2018Veröffentlichung Biota monitoring under the Water Framework Directive: On tissue choice and fish species selection(2018) Fliedner, Annette; Rüdel, Heinz; Koschorreck, Jan; Lohmann, NinaThe 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), ÎÌ-hexabromocyclododecane (ÎÌ-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, ÎÌ-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 ÎÌ-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. © 2017 The Authors. Published by Elsevier Ltd.Veröffentlichung Nutzung der Erfahrungen und Ergebnisse des Biotamonitorings der Umweltprobenbank für die Umsetzung des WRRL-Fischmonitorings(2019) Fliedner, Annette; Rüdel, Heinz; Koschorreck, JanDie Umweltprobenbank des Bundes (UPB) ist ein wichtiger Grundpfeiler der Umweltbeobachtung in Deutschland und ist bestrebt, die Länderbehörden bei neuen Anforderungen an das Umweltmonitoring zu unterstützen. So wurde eine Reihe von Studien durchgeführt, die für die Umsetzung des Wasserrahmenrichtlinien-Fischmonitorings von Interesse sind. Zum einen wurde die Wirksamkeit einer Datennormalisierung auf 26 % Trockenmasse (TM) oder 5 % Fettgehalt und Trophiestufe 4 (TS 4) erprobt, die im EU WRRL-Leitfaden Nr. 32 vorgeschlagen wird und dazu dienen soll, die Vergleichbarkeit heterogener Monitoringdaten zu erhöhen. Zum anderen wurde die Umrechnung von Schadstoffkonzentrationen im Filet auf Ganzfischkonzentrationen geprüft, um angepasste Risikobewertungen für Wildtiere und die menschliche Gesundheit zu ermöglichen. Darüber hinaus wurden die Einhaltung der Umweltqualitätsnormen (UQN) und die zeitlichen Verläufe der im Rahmen des WRRLFischmonitorings zu erfassenden organischen Stoffe an den 17 UPB-Messstellen (MS) in deutschen Flüssen und Seen untersucht. Die Ergebnisse zeigen, dass die Normalisierung von Quecksilber- und PFOS-Daten auf 26 % TM die Vergleichbarkeit unterschiedlicher Datensätze nicht erhöht. Eine Normalisierung auf 5 % Fett bei lipophilen Stoffen hatte dagegen deutliche Effekte. Eine Standardisierung auf TS 4, die sich auf Standardwerte für die Trophiestufen der Fische stützt und nicht auf tatsächlich gemessenen TS- Werte, führte nicht zu einer erhöhten Vergleichbarkeit zwischen verschiedenen Fischarten. Die UQN von Dicofol, HBCDD und HCB wurden von Brassen aller MS eingehalten, während flächendeckende Überschreitungen für PBDE beobachtet wurden. Die UQN-Einhaltung der übrigen Stoffe war abhängig vom Standort. An den meisten MS hat die Belastung der Fische seit Anfang der 2000er Jahre abgenommen. In: Korrespondenz Wasserwirtschaft : KW ; Organ der DWA ; Wasser, Boden, Natur - 12 (2019), Heft 6, Seite 336Veröffentlichung Levels, accumulation patterns and retrospective trends of perfluoroalkyl acids (PFAAs) in terrestrial ecosystems over the last three decades(2019) Falk, Sandy; Stahl, Thorsten; Fliedner, Annette; Koschorreck, JanAs a result of their ubiquitous presence in the environment perfluoroalkyl acids (PFAAs) have been demonstrated in numerous organisms worldwide, in particular in those of higher trophic levels. The fact that PFAAs have been detected in various human matrices, together with the resultant potential human health risks, knowledge of possible paths of entry and distribution in various ecosystems, is of great importance. In this context pooled samples of terrestrial ecosystems - roe deer liver (n=141), earthworms (n=44) as well as leaves from beech and poplar trees (n=70) - from the year 1989-2015 were obtained from the German Environmental Specimen Bank and examined for the presence of 11 PFAAs for the first time. In addition to determining individual and total PFAA concentrations, temporal trends have been deduced in order to determine the effectiveness of regulatory measures. The highest total mean concentration of PFAAs (sum of the concentrations of the 11 analytes) were 9.9 (Mü)g/kg in the roe deer liver samples, followed by earthworm samples with a mean PFAA concentration of 3.5 (Mü)g/kg and leaves with a mean total concentration of 2.5 (Mü)g/kg. In regard to temporal trends there was a significant reduction of concentrations for perfluorooctane sulfonate, perfluorooctanoic acid, perfluorononanoic acid and perfluorodecanoic acid in roe deer liver from 2003 to 2015, an indication of the effectiveness of regulatory measures. The same is true for the perfluorooctane sulfonate concentrations in earthworms and for perfluorooctanoic acid concentrations in the leaves. In contrast, an increase in perfluorobutanoic acid concentrations was observed from 2003 to 2015 in all three matrices. In summary it must be noted that in spite of the discernible effectiveness of minimization strategies, PFAAs are still detectable in terrestrial matrices and concentrations of other PFAAs as perfluorobutanoic acid appear to be increasing. Quelle: http://www.sciencedirect.comVeröffentlichung A field study in support of the monitoring of priority substances in German freshwater fish: derivation of fillet-to-whole fish conversion factors(2020) Rüdel, Heinz; Duffek, Anja; Radermacher, Georg; Fliedner, AnnetteBackground
Bioaccumulating contaminants in surface waters are preferably monitored in fish for assessing the related risks to and via the aquatic environment. Consequently, the European Water Framework Directive (WFD) requires a monitoring of certain priority substances such as mercury, polybrominated diphenyl ethers (PBDE), perfluorooctane sulfonic acid and its derivatives (PFOS), hexachlorobenzene (HCB), hexabromocyclododecanes (HBCDD) and polychlorinated dioxins/dioxin-like compounds (dioxins) in freshwater and coastal fish. Tissue levels have to comply with biota environmental quality standards (EQSs) given in Directive 2013/39/EU. EQSs are justified either by risks for human health (assessed on the basis of fillet) or secondary poisoning of wildlife (based on whole fish). To support the practical implementation of the WFD biota monitoring in Germany, comparative investigations of target fish species caught at six sites were performed.Results
At each site, at least three fish species listed in a national guidance document were sampled (e.g., chub, roach, bream, perch). Beside biometric data, concentrations of seven priority substances were determined in pooled fillet and carcass samples and whole fish data were calculated. The EQSs for PBDE and mercury were exceeded in nearly all fillet and whole fish samples. PFOS was above the EQS at several sites especially in perch, while HCB exceeded the EQS only at one site (Elbe River). All fillet and whole fish samples complied with the EQSs for dioxins and HBCDD. Based on wet weight concentrations of a homogeneous set of 20 composite sample pairs of 3â€Ì5 year-old fish, the following fillet-to-whole fish conversion factors were derived: mercury 0.81, PBDE 5.4, HCB 3.6, PFOS 2.7, dioxins 5.3, and HBCDD 1.8.Conclusions
Recommendations on selection of target fish species, age or tissue given by EU and national guidance documents are practical and feasible. However, further adjustments of the samplings such as the determination of site-specific length-age relationships are required from both ecological and risk assessment perspectives. The derived conversion factors allow the translation of fillet-to-whole fish concentrations (and vice versa), and thus the EQS compliance assessment for the appropriate tissue (fillet for human health, whole fish for wildlife risks) if only one tissue is investigated. Quelle: https://link.springer.comVeröffentlichung 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 Seasonal variability in metal and metalloid burdens of mussels: using data from the German Environmental Specimen Bank to evaluate implications for long-term mussel monitoring programs(2020) Knopf, Burkhard; Fliedner, Annette; Radermacher, Georg; Koschorreck, JanBackground Metal and metalloid concentrations in mussels can vary between seasons. In biota monitoring, the sampling time is therefore an important issue. Within the German Environmental Specimen Bank (ESB) program blue mussels (Mytilus edulis Complex) are sampled regularly since the 1980s. The samples are collected in two-monthly intervals at two North Sea sites and in 6-month intervals at one Baltic Sea site. All samples from one site and year are combined to annual composite samples and archived as sub-samples under cryogenic conditions. In order to investigate a possible reduction of the number of annual sampling intervals while maintaining comparability with the long-term composite sample data, the seasonal variability of metals/metalloids was analyzed based on the half-yearly and bimonthly samples of 2013, 2015 and 2017. Results In mussels from the North Sea site Eckwarderhoerne seasonality of metals/metalloids was comparable in all 3 years (arsenic being the only exception). At the North Sea site Koenigshafen seasonality of cobalt, nickel, cadmium, copper, lead, and arsenic was comparable in 2013 and 2015 but not in 2017, while selenium showed the same seasonality in all 3 years. Within 1 year, concentrations of metals and metalloids can vary by the same order of magnitude as observed between annual composite samples of different years making it impossible to select just one representative sampling time point per year that would provide the same information as the respective annual composite sample. Conclusions The findings highlight the importance of carefully selecting the sampling time point when using mussels in biota monitoring. For the German ESB program it is recommended to continue with the current sampling strategy and analyze annual composite samples in order to maintain comparability with the long-term data series, which are a special feature of the ESB. © The Author(s) 2020Veröffentlichung 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 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) 2020