German Environmental Specimen Bank Research Articles

The use of monitoring data in EU chemicals management--experiences and considerations from the German environmental specimen bank.

Since the 1970s, environmental specimen banks (ESB) have emerged in many countries. Their highly standardised sampling and archiving strategies make them a valuable tool in tracing time trends and spatial distributions of chemicals in ecosystem compartments. The present article intends to highlight the potential of ESBs for regulatory agencies in the European Union (EU). The arguments are supported by examples of retrospective monitoring studies conducted under the programme of the German ESB. These studies have evaluated the success of regulatory and industry provisions for substances of concern (i.e. PCB, polybrominated diphenyl ethers, perfluorinated compounds, alkylphenol compounds, organotin compounds, triclosan/methyl-triclosan, musk fragrances). Time trend studies revealed for example that levels of organotin compounds in marine biota from German coastal waters decreased significantly after the EU had decided on a total ban of organotin-based antifoulings in 2003. Similarly, concentrations of commercially relevant congeners of polybrominated diphenyl ethers decreased in herring gull eggs from the North Sea only after an EU-wide ban in 2004. The data presented demonstrate the usefulness of ESB samples for (retrospective) time trend monitoring and underline the benefit of a more intensive cooperation between chemicals management and specimen banking.

Journey into the past: using cryogenically stored samples to reconstruct the invasion history of the quagga mussel (Dreissena rostriformis) in German river systems

Knowledge about the spatial-temporal dynamics of biological invasions often remains incomplete, because precise information about the invaders' arrival dates is rare. This applies to the quagga mussel, which has become one of the most successful invasive species in Western European freshwaters. We here used cryogenically stored Dre- issena samples from the German Environmental Specimen Bank to reconstruct the colonization history of the quagga mussel in German river systems. Our retrospective genetic analysis significantly improved upon previous findings of when the quagga mussel arrived in Germany and can be used as chronological landmarks to reconstruct its range expansion. The discovery of Dreissena rostriformis in 2004 in the Rhine River near Koblenz presented the first record of this species not only in Germany, but also in Western Europe. Our results show that the quagga mussel had already invaded not only large parts of the Rhine and the Danube, but also the Elbe River. This demonstrates the value of cryobanked biological samples for the retrospective analysis of biological 'pollution' through alien invasive species.

Spatial and temporal trends of metals and arsenic in German freshwater compartments

Cadmium, lead, mercury, copper, nickel, zinc, and arsenic were analyzed in suspended particulate matter (SPM), zebra mussels, and bream sampled yearly under the program of the German Environmental Specimen Bank (ESB) in the rivers Rhine, Elbe, Danube, Saar, Mulde, and Saale and in Lake Belau. Temporal and spatial trends were analyzed, correlations between metal levels in different specimen types assessed, and sampling sites ranked according to their metal levels by calculating a Multi-Metal Index (MMI) for every specimen type and site. SPM: Highest metal loads were detected in Mulde, Saale, and Elbe right downstream of the Saale confluence. In the Elbe, metal loads in SPM were mostly highest in the upper and middle section of the river while in Rhine and Saar concentrations increased downstream. Temporal trends since 2005 were detected only at three sites. Zebra mussel: MMIs were highest in the tidal section of the Elbe and the lower Rhine and lowest in Lake Belau and the upper Danube. Different temporal trends were detected since the early 1990s depending on site and metal. Bream: As, Pb, Cu, and Hg were analyzed in muscle tissue and Pb, Cd, Cu, and Zn in liver. For both tissues, MMIs were highest in Mulde and Saale and the lower and middle Elbe. Since the early 1990s, Hg, Pb, and Cu decreased in bream muscle at many sites while As increased at 6 of the 17 sites. The findings indicate that Hg, Pb, and Cu have obviously decreased in many freshwater ecosystems in recent years, whereas As and Ni levels have increased at several sites. Metal levels and temporal trends mostly differed between the specimen types under investigation and only few correlations between specimen types were detected. This underlines the importance of including different components of an ecosystem when assessing its environmental quality.

The German Environmental Specimen Bank: Human Exposure to Perfluoroalkyl Substances – Time Trends and Inter-individual Variation

Background and aimsTo assess the impact of mitigation measures on the human exposure to perfluoroalkyl substances (PFAS) and to elucidate gender and other inter-individual differences, PFAS levels ...

Parabens and other phenols in urine samples of the German Environmental Specimen Bank (ESBHum) from 1995 to 2012: a retrospective exposure assessment

Because of the ubiquitous presence and the extensive use of parabensand other phenolic substances (like triclosan, triclocarban or benzophenones) in personal care and consumer products, food and beverage processing, pharmaceuticals and disinfectants humans are constantly exposed to these substances. Some of these substances are suspected to affect the endocrine system of humans. The German Environmental Specimen Bank (ESBHum) – supervised and scientifically coordinated by the German Federal Environment Agency (UBA) – archives human specimens since 1985 and thus allows assessing trends of human exposure. We quantified the body burden to these substances (9 parabens and 6 other phenolic substances) by analyzing 660 urine samples of the ESBHum (24h-urines) from the years 1995, 1997, 1999, 2001, 2003, 2005-2009 and 2012; 60 samples per year, from 30 male and 30 female volunteers (age: 21-29 years). We applied a newly developed highly sensitive on-line HPLC-MS/MS method, for the determination of these substances in urine. Analytical limits of quantification were in the range from 0.5 to 2 µg/L. The total concentration of the analytes (free and conjugated species) was measured. All samples were blinded before analysis. In nearly all samples parabens could be quantified.Median concentrations over the different years were around 40 µg/L for methyl-, 2 µg/L for ethyl- and 5 µg/L for n-propyl paraben. For the parabens this mainly reflects their consumption volume being highest for methyl paraben, followed by ethyl-, propyl- and butyl paraben. Triclosan was detected in around 60% of all samples analyzed. Median benzophenone-3 levels fell from around 2.5 µg/L (1995-2003) to < LOQ (2005-2012). For all other analytes medians are below the LOQ. Over the years we observed rather constant levels of exposures, except for the decrease in benzophenone-3. This retrospective study provides first data on internal exposures to the above substances in Germany from 1995 till 2012.

DINCH metabolites in urine samples of the German Environmental Specimen Bank (ESBHum) from 1999 to 2012: a retrospective exposure assessment

We analyzed 300 urine samples (24h voids) from the German Environmental Specimen Bank, for specific diisononylcyclohexane-1,2-dicarboxylate (DINCH) metabolites ranging from the simple monoester to several oxidized monoesters. Urine samples were collected in the years 1999, 2003, 2006, 2009 and 2012, 60 samples per year, from 30 male and 30 female volunteers (age: 21-29 years). The design of this retrospective study was chosen to investigate the time trend of DINCH exposure due to the market introduction of DINCH in 2002 and increasing production volumes ever since (to approx. 200,000 metric tons in 2012). The samples were analyzed by on-line HPLC-MS/MS with isotope dilution quantification. The LOQs for the oxidized DINCH metabolites are 0.05 µg/l and 0.1 µg/l for the monoester. All samples were blinded before analysis. We detected no DINCH metabolites in the 1999 and 2003 samples. From 2006 on the percentage of samples with DINCH metabolites above the LOQ increased significantly over the years (7% in 2006, 43% in 2009 and 98% in 2012). As expected, the hydroxyl monoester (OH-MINCH) was predominant followed by the carboxyl monoester (cx-MINCH) and the oxo monoester (oxo-MINCH). The median (and 95th percentile) of the OH-MINCH concentrations (in µg/L) increased from <LOQ (0.08) in 2006, to <LOQ (1.02) and 0.39 (2.09) in 2012. Similar trends, albeit at lower concentrations were observed for the other metabolites. All oxidized DINCH metabolites correlated strongly among each other over all concentrations spanning 4 orders of magnitude (rho>0.75, p>0.001). The median (95th percentile) DINCH intake in 2012 was calculated to be 0.14 (1.07) µg/kg body weight/day. Our results impressively show the advent and development of the exposure of the German population to DINCH since its market introduction in 2002. Daily intakes are still lower compared to the phthalates it is used for as a substitute; future measurements will enable us to monitor the development of exposure.

Entering markets and bodies: Increasing levels of the novel plasticizer Hexamoll® DINCH® in 24h urine samples from the German Environmental Specimen Bank

DINCH (diisononylcyclohexane-1,2-dicarboxylate) was introduced into the world market in 2002 as a non-aromatic plasticizer and phthalate substitute. We analyzed 300 urine samples (24 h voids) of the German Environmental Specimen Bank (ESB for Human tissues, ESB Hum) for specific DINCH metabolites by on-line HPLC-MS/MS with isotope dilution quantification. Urine samples of the ESB Hum were from the years 1999, 2003, 2006, 2009 and 2012, chosen to investigate the appearance and a possible trend of DINCH exposure since its market introduction. No DINCH metabolites were detected in the 1999 and 2003 samples. From 2006 on, the percentage of samples with DINCH metabolites above the LOQ increased significantly over the years (7% in 2006, 43% in 2009 and 98% in 2012). The cyclohexane-1,2-dicarboxylic acid-mono(hydroxy-isononyl) ester (OH-MINCH) was the predominant metabolite. Median (and 95th percentile) concentrations (in μg/l) increased from <LOQ (0.09) in 2006, to <LOQ (1.02) in 2009 to 0.39 (2.09) in 2012. All oxidized DINCH metabolites (OH-MINCH, cx-MINCH, oxo-MINCH) correlated strongly among each other (ρ>0.75, p<0.001). The median (95th percentile) DINCH intake in 2012 was calculated to be 0.14 (1.07)μg/kg body weight/day which is considerably below daily intakes currently deemed tolerable. DINCH is regarded to have a preferred toxicological profile over certain anti-androgenic phthalates. The continuation of DINCH measurements in the ESB Hum and other human biomonitoring studies like the German Environmental Survey (GerES) allows tracking the development of DINCH body burdens, the distribution of exposure levels and daily intakes, providing basic data for future toxicological assessment and further epidemiological studies.

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

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 <0.2–3.4ngg−1ww (wet weight; corresponding to <2–69ngg−1lw, lipid weight) without apparent concentration trends over time. MTCS was detected at considerably higher concentrations in fish ranging from 1.0–33ngg−1ww (47–1010ngg−1lw) 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 1–4ngg−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.

Derivation of dynamic reference values for the classification of contaminant concentrations in bream (Abramis brama) of German rivers and lakes using data of the Environmental Specimen Bank

A direct assessment of contaminant concentrations in biota with respect to their biological relevance or importance for the ecosystem is rarely possible. Statistically derived reference values can serve as a guide to classify measured tissue concentrations, but they do not provide any information on the biological significance of the contaminant concentrations. However, previously such reference values did not exist for environmental-biomonitoring. Based on analytical data from muscle tissue of bream (Abramis brama) of the German Environmental Specimen Bank (ESB), we present a method on how to derive dynamic reference values. These show the general state of inland surface water pollution in Germany at a certain time. The reference values allow for classification of measured contaminant concentrations in muscle tissue of bream. This classification enables a comparative assessment in means of how the actual state of pollution in a specific ecosystem is, compared to the general, macro state of pollution.

Retrospective monitoring of perfluorocarboxylates and perfluorosulfonates in human plasma archived by the German Environmental Specimen Bank

Due to the increased awareness of the ubiquitous contamination of all environmental compartments and of human beings with perfluoroalkyl substances (PFAS), voluntary withdrawals and shifts in products and manufacturing technologies, as well as in regulatory measures, have been made. To investigate whether these activities are reflected in the human exposure to PFASS, we examined human blood archived by the German Environmental Specimen Bank. Plasma samples (n=258, age range 20-29 years) covering the observation period 1982-2010 were analyzed for eleven perfluoroalkylcarboxylates (C4-C14) and five perfluoroalkylsulfonates (C4-C10) by HPLC-MS-MS. We detected perfluorooctanesulfonate (PFOS), perfluorooctanoate (PFOA), and perfluorohexanesulfonate (PFHxS) most often of all PFASs. Following a sharp increase from 1982 to 1986, median PFOS concentrations remained in the range of 20-24ng/mL until the end of the 1990s. Between 2001 and 2010, PFOS concentrations decreased steadily to 4ng/mL in plasma. Except for a similar strong increase from 1982 to 1986, we observed PFOA concentrations fluctuating between 4.8 and 6.3ng/mL in the following years. Since 2008, ESB data suggest a decreasing trend of PFOA. PFHxS concentrations increased continuously between 1982 and 2001 from about 1-2ng/mL. After nearly unchanged concentrations until 2005, a downward trend of PFHxS in plasma became apparent and in 2010 resulted in levels which were about 20% lower than those observed in the early 1980s. In the case of shorter and longer chained PFASs, quantification frequencies were between 0 and 60% and we found no indication of any temporal trends in human plasma concentrations.

Bisphenol A in 24 h urine and plasma samples of the German Environmental Specimen Bank from 1995 to 2009: A retrospective exposure evaluation

Human exposure to Bisphenol A (BPA) is omnipresent. Both the extent of the exposure and its toxicological relevance are controversially discussed. We aim to reliably determine and evaluate the extent of BPA body burden in the German population from 1995 to 2009 based on 600 24 h urine samples and corresponding plasma samples from the Environmental Specimen Bank. We determined total and unconjugated BPA in urine and plasma using on-line solid-phase extraction high-performance liquid chromatography coupled to isotope dilution tandem mass spectrometry with a limit of quantification (LOQ) of 0.1 μg/l. In the stored urines, total BPA was quantifiable in >96% (median: 1.49 μg/l; 95th percentile: 7.37 μg/l), whereas unconjugated BPA was quantifiable only in <15% of the samples. Total BPA concentrations decreased over time, but 24 h urine volumes increased. Therefore, daily intakes calculated from the 24 h urines remained rather constant at a median of 0.037 and a 95th percentile of 0.171 μg BPA/kg body weight/day. In 60 corresponding plasma samples, total BPA levels were generally below the LOQ of 0.1 μg/l and, if quantifiable, most BPA was unconjugated, thus hinting to external contamination. We see total BPA in urine as the most appropriate and robust marker for BPA exposure assessment (if controlled for BPA contamination). Unconjugated BPA in urine and unconjugated or total BPA in plasma where contamination or breakdown of the glucuronide cannot be ruled out are of no value for human exposure assessment.

Environmental surveys, specimen bank and health related environmental monitoring in Germany

Production of chemicals, use of products and consumer goods, contamination of food as well as today's living conditions are related to a substantial exposure of humans to chemicals. Safety of human beings and the environment has to be safeguarded by producers and government. Human biomonitoring (HBM) has proven to be a useful and powerful tool to control human exposure and facilitate risk assessment. Therefore, the German Federal Environment Agency (Umweltbundesamt, UBA) employs two major HBM tools, the German Environmental Survey (GerES) and the German Environmental Specimen Bank (ESB). GerES is a nationwide population representative study on HBM and external human exposure, which has, inter alia, been used to identify lead in tap water, lead dustfall, time spent in traffic, and age of dwelling as exposure sources for lead and, thus, to derive risk reduction measures. The ESB is a permanent monitoring instrument and an archive for human specimens. Retrospective monitoring of phthalates and bisphenol A provides a continuous historical record of human exposure in Germany, over the last decades. Additionally it revealed that estimations of human exposure based on production and consumption data may supply misleading information on human exposure. HBM data demonstrated that (a) the use if the restricted isomer di-n-butylphthalat decreased while di-i-butylphthalate levels remained constant and (b) human bisphenol A exposure might be overestimated without monitoring data. The decrease of polycyclic aromatic hydrocarbon-exposure proves the success of German environmental policy after German re-unification. In addition to GerES and ESB UBA is involved in different co-operation networks, the two most prominent of which are (1) the harmonization of HBM in Europe (ESBIO; Expert Team to Support Biomonitoring in Europe, COPHES/DEMOCOPHES; Consortium to Perform Human Biomonitoring on a European Scale/Demonstration of a study to Coordinate and Perform Human Biomonitoring on a European Scale) and (2) the co-operation between BMU and the German Chemical Industry Association (VCI). In the latter project emphasis will be placed on substances with a potential relevance for health and on substances to which the general population might potentially be exposed to a considerable extent and for which HBM methods are not available up to now.

Human and environmental biomonitoring of polychlorinated biphenyls and hexachlorobenzene in Saxony, Germany based on the German Environmental Specimen Bank

The objective of the present study was to investigate the principle relationships between concentrations in human and environmental matrices of polychlorinated biphenyls (PCBs) and hexachlorobenzene (HCB) in short distance comparable areas within Saxony, Germany by employing the data of the German Environmental Specimen Banking (ESB). Examples supporting this idea were presented by selecting data on blood plasma collected from students in University of Halle and pine shoots, egg matter of city pigeons, earthworm, and roe deer liver. Similar pattern for PCB 138 and PCB 180 was found for the human plasma and pine shoots samples during investigated years and the human data followed the corresponding environmental levels with some delay of approximately two years. However, PCB 153 that was the prevailing congener did not manifest this relationship. In addition, the correlation of the ratios of concentrations (human/environmental concentration) to some physicochemical constants such as molecular weight (MW), octanol-water partition coefficient (logK(ow)), Henry's law constant (K(H)), and sorption partition coefficient (logK(oc)) of HCB, PCB 138, PCB 153, and PCB 180 were studied. The resulted negative slopes with all constants in case of blood plasma/city pigeons egg matter pairs suggested that the accumulation of lipophilic compounds is more pronounced in pigeon eggs than in human blood.

Survey of patterns, levels, and trends of perfluorinated compounds in aquatic organisms and bird eggs from representative German ecosystems

Samples from the German Environmental Specimen Bank (ESB) covering particularly the years 1994-1996, 2000-2002, and 2006-2009 were analyzed for perfluorinated compounds (PFC; mainly C4-C13 carboxylic and sulfonic acids) to gain an overview on current PFC levels and patterns in marine, limnetic, and terrestrial biota; to assess their concentrations in different trophic levels; and to investigate whether risk management measures for PFC are successful. Specimens, either standardized annual pooled samples (blue mussels, eelpout liver, bream liver, pigeon eggs) or individual single samples (cormorant eggs, rook eggs), were collected for the German ESB program from representative sampling sites according to documented guidelines. After appropriate extraction, PFC were quantified under ISO/IEC 17025 accreditation by HPLC/MS-MS with isotopically labeled internal standards. Limits of quantification (LOQs) were 0.2-0.5 ng/g. Data are reported on a wet weight basis. In most samples the predominant PFC was perfluorooctane sulfonic acid (PFOS). However, in marine mussels from North and Baltic Seas, PFOS levels were mostly below the LOQ, but low residues of PFOS amide were found which declined in recent years. Livers of eelpout showed maximum concentrations of 15-25 ng/g PFOS in the period 2000-2002 and low amounts of perfluoropentanoate in all years. Beside PFOS (median 48 ng/g) several PFC could be determined in cormorant eggs sampled in 2009 from a Baltic Sea site. For a freshwater ecosystem, current PFC burdens for cormorant eggs were even higher (median 400 ng/g PFOS). Livers of bream from rivers showed concentrations of 130-260 ng/g PFOS, but for bream from a reference lake levels were only about 6 ng/g. In contrast to cormorants, eggs of rook and feral pigeon from terrestrial ecosystems displayed only low PFC burdens (up to 6 ng/g PFOS). Generally, PFC levels were lower in marine than in freshwater biota. PFC burdens were higher in biota from the ESB-North Sea sites than in Baltic Sea organisms. Levels of PFC were quite high especially in top predators of both limnetic and marine ecosystems. Only low PFC levels were detected in eggs of terrestrial birds. A decrease of PFOS levels from maximum values around the year 2000 observed at least in North Sea biota may be a result of a production cease and shifts in marketing pattern.

Use of sex ratio of bream ( Abramis brama L.) as an indicator of endocrine effects: Results from the German Environmental Specimen Bank

In field monitoring, sex ratio as an endpoint of possible endocrine effects at population level can only be recorded as the deviation from the natural sex ratio. Unfortunately, data on natural sex ratios of many species cannot be used to control for such effects. This also applies to bream ( Abramis brama L.), an important fish species in passive biomonitoring. Here we show that in natural bream populations the sex ratio decreases with increasing age. Age class specific correction coefficients were derived to eliminate age-dependency of the sex ratio.

The potential of spatial information in human biomonitoring by example of two German environmental epidemiology studies

This study aimed at statistically investigating the association between the internal exposure of children and young adults to uranium (U) and epidemiologically relevant external determinants of exposure. The investigation was performed with data from two studies within the framework of the German health-related environmental monitoring program: The German Environmental Survey for Children (GerES IV) conducted by the Federal Environment Agency (Umweltbundesamt) with data on 1,780 children 3-14years of age and their home environment and the German Environmental Specimen Bank (ESB, section: human specimens) with data on 2,253 students 20-29years of age. Both studies provided data on the U levels in human urine for all probands. GerES IV furthermore provided an extensive environmental and demographic database on, e.g., U levels in drinking water. The data from GerES IV and ESB were linked by GIS to spatially relevant exposure information, including background values of U in stream sediments and in upper and lower soils, U levels in mosses and particulate matter in the lower atmosphere, precipitation and elevation as well as forest density. Bivariate correlation analysis and two decision tree models showed moderate but significant associations between U in human urine and U levels in drinking water, stream sediments and upper and lower soils. Future investigations considering additional epidemiologically relevant data sets may differentiate the results. Furthermore, the sample design of future environmental epidemiology studies should take the spatial evaluation of the data into greater account.

Temporal trend (1988–2008) of hexabromocyclododecane enantiomers in herring gull eggs from the german coastal region

Levels of α-, β-, and γ-hexabromocyclododecane (HBCD) were determined in pooled eggs from herring gulls ( Larus argentatus) sampled on three bird sanctuaries near the German North Sea coast between 1988 and 2008 (Mellum and Trischen) and the German Baltic Sea coast between 1998 and 2008 (Heuwiese) and archived by the German Environmental Specimen Bank. Pressurized fluid extraction, gel permeation chromatography, and LC–MS/MS using 13C 12-labelled isotope standards and a chiral column were applied. α-HBCD was the dominating diastereomer and ranged between 3.7 and 107 ng g −1 lw while β- and γ-HBCD were throughout close to LOQ. The highest α-HBCD concentration was found in eggs from Mellum sampled in the year 2000. Interestingly, HBCD in eggs from the three islands displayed similar time courses with levels increasing to a peak contamination around 2000 and decreasing levels ever since. Chiral signatures of α-HBCD in eggs differed among the islands but indicated a preferential enrichment of the first eluting enantiomer (−)-α-HBCD.

The German Environmental Specimen Bank—An integrative Tool for Human and Environmental Monitoring in Chemical Risk Assessment

The German Environmental Specimen Bank—An integrative Tool for Human and Environmental Monitoring in Chemical Risk Assessment

Workshop of the German Environmental Specimen Bank on monitoring of priority pollutants and emerging substances in sewage sludge

Workshop of the German Environmental Specimen Bank on monitoring of priority pollutants and emerging substances in sewage sludge

Twenty years of elemental analysis of marine biota within the German Environmental Specimen Bank--a thorough look at the data.

As one component of the German ecological environment observation, the Environmental Specimen Bank program was initiated in the mid-1980s. Under the program, representative specimens of marine, fresh water, and terrestrial ecosystems are sampled regularly and archived under chemically stable conditions. An initial characterization of the samples provides data regarding the status quo of the respective ecosystems. The aim of the present publication is to give insight into these real-time monitoring data, which have been generated for the last 10 to 20 years. This is done exemplarily for the heavy metals cadmium (Cd), mercury (Hg), and lead (Pb) in marine specimens of the Baltic and the North Sea. Bladder wrack (Fucus vesiculosus), blue mussel (Mytilus edulis), eelpout (Zoarces viviparus), and eggs of herring gulls (Larus argentatus) were sampled at one location in the Baltic Sea and at two sites in the North Sea (Schleswig-Holstein Wadden Sea and Lower Saxony Wadden Sea). Annual samples were pooled, homogenized, and analyzed for a set of elements. Cd and Pb were quantified after freeze-drying and microwave digestion using inductively coupled plasma-mass spectrometry. Total Hg in freeze-dried samples was determined by atomic absorption spectrometry using a direct mercury analyzer. Time series data covering up to two decades revealed comparable cadmium levels at all three locations. Concentrations in bladder wrack ranged between 0.10 and 0.37 microg/g on a wet weight basis (ww). Respective values for blue mussel and eelpout liver were 0.07-0.29 and 0.01-0.10 microg/g ww. Herring gull eggs were not included in cadmium analyses. Declining trends were observed in North Sea bladder wrack and mussels, eelpout from the Lower Saxony site, and mussels from the Baltic Sea. Upward trends were apparent in eelpout from the Schleswig-Holstein location. Mercury concentrations in Baltic Sea specimens ranged from 1.1-2.7 ng/g ww in bladder wrack to 2.6-5.1, 26-52, and 86-226 ng/g ww in blue mussel, eelpout muscle, and herring gull eggs, respectively. No temporal trends were observed. North Sea bladder wrack had accumulated 5.4-24 ng/g ww Hg. The respective Hg values for blue mussel and eelpout muscle were 19-64 and 73-187 ng/g ww. Highest Hg contents were detected in herring gull eggs (90-1,100 ng/g ww). Declining trends of Hg were observed in herring gull eggs at both North Sea locations and in blue mussels at the Lower Saxony site. Lead concentrations in Baltic Sea specimens were 48-222 ng/g ww in bladder wrack, 85-189 ng/g ww in blue mussel, 2.0-9.5 and 10-42 ng/g ww in eelpout muscle and liver, and 2.7-26 ng/g ww in herring gull eggs. In the North Sea, Pb concentrations were as follows: 68-397 ng/g ww in bladder wrack, 101-507 ng/g ww in blue mussels, 2.6-35 and 5.9-158 ng/g ww in eelpout muscle and liver, and 3.5-55 ng/g ww in herring gull eggs. Highest Pb-levels were found at the Lower Saxony site. Declining Pb-trends were observed in bladder wrack from the Baltic Sea; in bladder wrack and mussel at the Schleswig-Holstein location; and in bladder wrack, mussels, eelpout liver, and herring gull eggs at the Lower Saxony site. During the 10 to 20 years of monitoring, reliable data were obtained which allow a good insight into metal contamination of marine biota. Assessment of the data according to OSPAR criteria (OSPAR 2005) revealed cadmium levels above the derived background concentrations in mussels of all three sites. Mercury levels above background concentrations were found at both North Sea locations, whereas only mussels at the Lower Saxony site had Pb concentrations above the reference value. Archived specimens are available for further analyses and questions which may arise in the future (speciation of elements, metallomics).