Person: Koschorreck, Jan
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Veröffentlichung Long-term data for PFAS in soils from German ecosystems, including TOP assay(2023) Bandow, Nicole; Koschorreck, Jan; Wellmitz, JörgIn this study, soil top layers from the German Environmental Specimen Bank (ESB) covering a period from 2002 to 2018 and 11 sampling sites representing four ecosystem types were analysed for 24 PFAS (11 PFCA, 7 PFSA, and 6 precursors), including the total oxidizable precursor (TOP) assay. Median (Sigma)PFAS levels before and after TOP assay ranged from 0.31 to 19.7 (micro)g/kg dry weight (dw) and 0.32 to 20.4 (micro)g/kg dw, respectively. The most frequently measured PFAS above LOQ were PFOS and PFOA, which were present at concentrations above 0.1 (micro)g/kg dw in each sample. Both accounted, on average, for half to two-thirds of the total identified PFAS load at most sites. The investigated samples from the near-natural and forestry ecosystem types each had significantly higher PFAS levels than those from the urban-industrial ecosystem type, while samples from the agricultural ecosystem type did not differ distinctly from the others. Increases of median ΣPFAS levels after TOP assay ranged up to slightly >20 %, indicating that precursor compounds do not play a major role in the substance spectrum of German ESB soil samples from different ecosystem types. Total organic carbon (TOC) content in analysed samples ranged from about 1 % in sandy soil to >40 % in litter layer and showed a strong positive correlation with PFAS concentrations. It is therefore highly recommended that TOC content is reported along with PFAS levels in soils. PFAS trend analysis for nine sampling sites before and after TOP assay showed that concentration levels at most sites have remained more or less stable for the sampled period of almost two decades. The constant PFAS levels in soil samples indicate that PFOS and PFOA regulations have not yet had a positive effect on the exposure situation in this environmental compartment. ©2023 The Authors.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 Trends for plasticizers in German freshwater environments - Evidence for the substitution of DEHP with emerging phthalate and non-phthalate alternatives(2020) Koschorreck, Jan; Nagorka, ReginePlasticizers are marketed in high volumes and Di(2-ethylhexyl) phthalate (DEHP) is frequently detected in the environment and human populations. Industry had largely relied on DEHP until regulation started to restrict its marketing in 1999 due to environmental and human health concerns. The aim of this study was to obtain spatial-temporal trends for DEHP and its substitutes in German rivers. We have investigated suspended particulate matter (SPM) samples from the German Environmental Specimen Bank (ESB) for the presence of 23 plasticizers, i.e. 17 phthalates and 6 non-phthalates. The samples were collected in the last 10 years at 13 sites in large river basins in Germany such as the Rhine, Elbe and Danube. A decrease in DEHP concentrations was observed at all sampling sites between the mid-2000s and 2017. The maximum concentration for DEHP was determined in 2006 in samples from Rehlingen/Saar (6720 ng/g dry weight (dw)). By 2017, the DEHP concentration in Rehlingen had dropped to 2080 ng/g dw. Currently, Diisononyl phthalate (DINP) is the plasticizer with the highest levels in the SPM samples (maximum value 4150 ng/g dw in Rehlingen/Saar). Our results show that novel plasticizers such as Diisononylcyclohexane-1,2-dicarboxylate (DINCH) spread rapidly in surface waters after their market introduction. We have found several plasticizers of emerging concern in the environmental samples, the further use of which is currently under review under the EU chemicals regulation (REACH, registration, evaluation, authorisation and restriction of chemicals). In particular for Di(2-propylheptyl) phthalate (DPHP) a significant increase in concentration was observed at almost all sites between the mid-2000s and 2017, for example in Prossen/Elbe from 24 ng/g dw (2005) to 1380 ng/g dw (2017). © 2020 The Authors.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 Spatial distribution and temporal trends of pharmaceuticals sorbed to suspended particulate matter of German rivers(2020) Boulard, Lise; Dierkes, Georg; Schlüsener, Michael P.; Koschorreck, JanAlthough several studies confirmed a wide distribution of pharmaceuticals in rivers and streams, a limited knowledge is available about the partitioning of pharmaceuticals between the water phase and suspended particulate matter (SPM). To close this gap of knowledge, we developed and validated a sensitive and high throughput analytical method for the analysis of 57 pharmaceuticals, 42 metabolites and transformation products (TP) as well as the artificial sweetener acesulfame sorbed to SPM. The method was based on pressurized liquid extraction (PLE) followed by a clean-up via solvent exchange and detection via direct injection-reversed phase LC-MS/MS and freeze-drying-HILIC-MS/MS. Freundlich isotherms were determined for 90 analytes. All showed a linear sorption behavior. Distribution coefficients (Kd) ranged from 0.64 L/kg to 9300 L/kg. For 18 pharmaceuticals, Kd values were found to be above 100 L/kg. SPM of annual composite samples were analyzed to determine the pharmaceutical concentrations between 2005 and 2015 at four sites of the river Rhine: Weil, Iffezheim, Koblenz and Bimmen as well as between 2006 and 2015 at one site of the river Saar, at Rehlingen. In these SPM samples, up to 61 of the 100 analytes were detected with concentrations up to 190 ng/g d.w. (dry weight) for guanylurea, a transformation product of the antidiabetic metformin. For most analytes, increasing concentrations were found along the length of the Rhine and higher concentrations were measured in Rehlingen/Saar. Normalization of the data with the antiepileptic drug carbamazepine as an intrinsic tracer for municipal wastewater indicated possible industrial discharges for four analytes. For most pharmaceuticals, the annual concentrations exhibited a good correlation with the consumption volumes in Germany. © 2019 Published by Elsevier Ltd.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 Hg isotopic composition of one-year-old spruce shoots: Application to long-term Hg atmospheric monitoring in Germany(2021) Yamakawa, Akane; Amouroux, David; Fettig, Ina; Tessier, Emmanuel; Koschorreck, JanThe Hg isotopic composition of 1-year-old Norway spruce (Picea abies) shoots collected from Saarland cornurbation Warndt, Germany, since 1985 by the German Environmental Specimen Bank, were measured for a better understanding of the temporal trends of Hg sources. The isotopic data showed that Hg was mainly taken up as gaseous element mercury (GEM) and underwent oxidation in the spruce needles; this led to a significant decrease in the δ202Hg compared with the atmospheric Hg isotopic composition observed for deciduous leaves and epiphytic lichens. Observation of the odd mass-independent isotopic fractionation (MIF) indicated that ÎÌ199Hg and ÎÌ201Hg were close to but slightly lower than the actual values recorded from the atmospheric measurement of the GEM isotopic composition in non-contaminated sites in U.S. and Europe, whereas observation of the even-MIF indicated almost no differences for ÎÌ200Hg. This confirmed that GEM is a major source of Hg accumulation in spruce shoots. Interestingly, the Hg isotopic composition in the spruce shoots did not change very significantly during the study period of >30 years, even as the Hg concentration decreased significantly. Even-MIF (ÎÌ200Hg) and mass-dependent fractionation (MDF) (δ202Hg) of the Hg isotopes exhibited slight decrease with time, whereas odd-MIF did not show any clear trend. These results suggest a close link between the long-term evolution of GEM isotopic composition in the air and the isotopic composition of bioaccumulated Hg altered by mass-dependent fraction in the spruce shoots. © 2021 The AuthorsVeröffentlichung Umweltprobenbank des Bundes(Umweltbundesamt, 2022) Badry, Alexander; Bandow, Nicole; Fettig, Ina; Körner, Andrea; Koschorreck, Jan; Künitzer, Anita; Nagorka, Regine; Rüther, Maria; Weber, Till; Wellmitz, Jörg; Deutschland. UmweltbundesamtDieser Bericht fasst die wesentlichen Arbeiten der Umweltprobenbank des Bundes im Jahr 2020 zusammen. Die Umweltprobenbank des Bundes unterstützt die Umsetzung des Vorsorgeprinzips mit einer wissenschaftlichen Infrastruktur, einer umfassende Datenbasis zur Bestimmung und Bewertung des Ist-Zustandes der Umwelt und einer langfristigen Beobachtung der in der Umwelt stattfindenden chemischen, physikalischen und biologischen Entwicklungsprozesse. Dafür sammeln Fachleute Humanproben ausgewählter Standorte gemeinsam mit ökologisch repräsentativen Umweltproben, archivieren sie bei tiefkalten Temperaturen und führen Untersuchungen auf gesundheits- und umweltrelevante Stoffe durch. Auf diese Weise wird auch eine Kontrolle der Wirksamkeit umweltpolitischer Maßnahmen möglich, beispielsweise bei Beschränkungen der Verwendung von Stoffen. Quelle: www.umweltbundesamt.deVeröffentlichung Quaternary Alkylammonium Disinfectants in suspended particulate matter of German rivers before and during the SARS-CoV-2 Pandemic(2022) Balachandran, Sanjana; Lennartz, Sophie; Glaeser, Stefanie P.; Koschorreck, JanVeröffentlichung Long-term trends for blue mussels from the German Environmental Specimen Bank show first evidence of munition contaminants uptake(2023) Strehse, Jennifer Susanne; Bünning, Tobias; Koschorreck, Jan; Künitzer, AnitaSubmerged munitions are present in marine waters across the globe. They contain energetic compounds (ECs), such as TNT and metabolites thereof, which are considered carcinogenic, exhibit toxic effects in marine organisms, and may affect human health. The aim of this study was to investigate the occurrence of ECs and their trends in blue mussels from the annual collections of the German Environmental Specimen Bank sampled over the last 30 years at three different locations along the coastline of the Baltic and North Sea. Samples were analyzed by GC-MS/MS for 1,3-dinitrobenzene (1,3-DNB), 2,4-dinitrotoluene (2,4-DNT), 2,4,6-trinitrotoluene (TNT), 2-amino-4,6-dinitrotoluene (2-ADNT), and 4-amino-2,6-dinitrotoluene (4-ADNT). The first signals indicating trace levels of 1,3-DNB were observed in samples from 1999 and 2000. ECs were also found below the limit of detection (LoD) in subsequent years. From 2012 onwards, signals just above the LoD were detected. The highest signal intensities of 2-ADNT and 4-ADNT, just below the LoQ (0.14 ng/g d.w. and 0.17 ng/g d.w., respectively), were measured in 2019 and 2020. This study clearly shows that corroding submerged munitions are gradually releasing ECs into the waters that can be detected in randomly sampled blue mussels, even though the concentrations measured are still in the non-quantifiable trace range. © Authors