Die Punktdarstellung (WMS) zeigt Proben aus dem BGR-Erdölarchiv, die für die Bundesrepublik Deutschland an der Bundesanstalt für Geowissenschaften und Rohstoffe (BGR) vorliegen. Sie zeigt die Standorte und ausgewählte Informationen zur Bohrung, wie den Bohrungsnamen und den NIBIS-BohrIdentifier (NIBIS Kartenserver des Landesamtes für Bergbau und Geologie Niedersachsens). Die Erdöle liegen in unterschiedlichen Mengen vor und werden in der Regel gekühlt gelagert. Zu vielen Proben hält die BGR geochemische Daten vor, wie relative Anteile an aliphatischen und aromatischen Bestandteilen, die isotopische Zusammensetzung (delta13C) von Erdölfraktionen und Verhältnisse ausgewählter aliphatischer Kohlenwasserstoffe und Biomarker (speziell Sterane und Hopane). Proben sowie Daten sind nur nach rechtlicher Klärung durch den Bohrungsbesitzer möglich. Eine Kontaktherstellung durch die BGR ist möglich.
Die Punktdarstellung zeigt Proben aus dem BGR-Erdölarchiv, die für die Bundesrepublik Deutschland an der Bundesanstalt für Geowissenschaften und Rohstoffe (BGR) vorliegen. Sie zeigt die Standorte und ausgewählte Informationen zur Bohrung, wie den Bohrungsnamen und den NIBIS-BohrIdentifier (NIBIS Kartenserver des Landesamtes für Bergbau und Geologie Niedersachsens). Die Erdöle liegen in unterschiedlichen Mengen vor und werden in der Regel gekühlt gelagert. Zu vielen Proben hält die BGR geochemische Daten vor, wie relative Anteile an aliphatischen und aromatischen Bestandteilen, die isotopische Zusammensetzung (delta13C) von Erdölfraktionen und Verhältnisse ausgewählter aliphatischer Kohlenwasserstoffe und Biomarker (speziell Sterane und Hopane). Proben sowie Daten sind nur nach rechtlicher Klärung durch den Bohrungsbesitzer möglich. Eine Kontaktherstellung durch die BGR ist möglich.
As tools for environmental monitoring of pharmaceuticals, mode of action -based in vitro-assays were developed for beta-blockers as metoprolol, and non-steroidal anti-inflammatory drugs, as diclofenac. In order to validate these tests for their suitability to reflect in vivo-effects in aquatic organisms, toxicity tests and biomarker studies were conducted with fish, crustaceans, snails and sediment-dwelling invertebrates. Test were conducted in laboratory, aquatic mesocosm and under field conditions. In addition to population relevant endpoints individual health parameters were determined by means of stress protein analyses, histological investigations and studies revealing oxidative stress. Veröffentlicht in Texte | 44/2017.
For the evaluation of effects of hormone-active substances to fish, several test guidelines have been validated by the OECD which are included in the Conceptual Framework for Testing and Assessment of Endocrine Disruptors (OECD, 2010). In these tests, the assessment of physiological parameters is limited to the established biomarkers like vitellogenin or 11-keto testosterone in blood plasma or liver tissue. A promising approach to refine existing testing strategies is the integration of molecular endpoints, which rapidly respond to exposure. Furthermore, these endpoints can be indicative of potential adverse effects at the organismal level by providing information, which connect to the initiating effect of a substance. This is in line with the concept of Adverse Outcome Pathways (AOP), which evolved from the “toxicity pathway” approach as a mechanistic evaluation tool for the risk assessment. Veröffentlicht in Texte | 41/2016.
Schmidtkunz, Christoph; Gries, Wolfgang; Weber, Till; Leng, Gabriele; Kolossa-Gehring, Marike International Journal of Hygiene and Environmental Health (2019), online 14. Februar 2019 Di(2-propylheptyl) phthalate (DPHP) is used as a substitute for high molecular weight phthalates like di(2-ethylhexyl) phthalate (DEHP) which were subjected to authorization under REACh in 2015. An earlier study on the time trend of exposure in human 24-h urine samples from the German Environmental Specimen Bank has revealed that metabolites of DPHP emerged in 2009 and 2012 (Schütze et al., 2015). In order to better assess a potential trend and the present state of exposure to DPHP, we now measured 180 urine samples from the German Environmental Specimen Bank, 60 per year, collected in 2011, 2014 and 2017, randomized and blinded before analysis. Together with the previously analyzed samples, data for a total of 480 samples covering 19 years from 1999 to 2017 was thus generated. We were able to show that DPHP exposure of the studied population, university students from Münster (Northwestern Germany), has remained essentially constant since 2011, after a rapid increase starting around 2009. Even so, urinary metabolite concentrations were always in the low ppb or sub-ppb range, indicating that DPHP exposure of the general population is substantially lower than for other modern plasticizers, and far below levels currently regarded as critical. DPHP is a plasticizer which is mostly used in non-sensitive applications with little probability of close contact to humans. Still, we observed how temporal trends of DPHP exposure largely follow trends of DPHP consumption in the Western European market. Our results hence demonstrate the potential of biomonitoring to sensitively detect the effects of industrial product strategy on the environment, even when biomarkers are present only at trace level. doi: 10.1016/j.ijheh.2018.12.008
Scherer, Max; Petreanu, Wolf; Weber, Till; Scherer, Gerhard; Pluym, Nikola; Kolossa-Gehring, Marike Chemosphere (2020), 128955; online 12. November 2020 2-(4-tert-butylbenzyl)propionaldehyde (trade names, e.g. lysmeral or lilial) is a fragrance chemical frequently used in cosmetic products where it is labelled as Butylphenyl methylpropional. A recently developed LC-MS/MS method for the analysis of four lysmeral metabolites (tert-butylbenzoic acid (TBBA), lysmerol, lysmerylic acid, and hydroxy-lysmerylic acid) was applied to 329 urine samples from the Environmental Specimen Bank collected between 2000 and 2018. The two major metabolites TBBA and lysmerol were found in quantifiable concentrations in almost all samples in this study and correlated significantly. Hence, both analytes proved to be specific biomarkers indicating the broad exposure to lysmeral. A significant decline was found for TBBA and lysmerol for the monitored years with the most pronounced decrease from 2012 to 2015. The daily intake (DI) was used to evaluate potential health risks with respect to the derived no-effect level (DNEL) as a threshold for exposure of the general population. The median DI (1.63 μg/kg bw/d) and the 95th percentile (4.69 μg/kg bw/d) corresponded to 2.6% and 7.5% of the lowest DNEL (62.5 μg/kg bw/d for oral administration), respectively. Even though a decreasing trend in exposure was observed the data still calls for efforts to reduce the exposure towards lysmeral since metabolites of lysmeral were detected in nearly all samples and adverse effects cannot be excluded. Clearly, these results need to be substantiated by HBM campaigns in population representative samples like the German Environmental Survey in adults (GerES VI) to provide more robust data for the adult population. doi: 10.1016/j.chemosphere.2020.128955
Pluym, Nikola; Stöckelhuber, Markus; Weber, Till; Scherer, Gerhard; Scherer, Max; Kolossa-Gehring, Marike International Journal of Hygiene and Environmental Health 239 (2022), 113880; online 10. November 2021 Geraniol (trans-3,7-dimethyl-2,6-octadiene-1-ol) is an acyclic isoprenoid monoterpene with a widespread use as fragrance in consumer products, agrochemicals and pharmaceuticals. The class of terpene chemicals has been associated with varying sensitizing potencies. A recently developed sensitive LC- MS/MS method for the analysis of geraniol metabolites was further improved and validated for the two metabolites, 8-carboxygeraniol and Hildebrandt acid. The successfully validated method was applied to 250 urine samples derived from the Environmental Specimen Bank (ESB) collected between 2004 and 2018. Both metabolites of this allergen of special concern were quantified in all urine samples of this study. Correlation analysis revealed that 8-carboxygeraniol appears to be the sole specific biomarker in urine for geraniol exposure. Overall, the excreted amounts of 8-carboxygeraniol remained unchanged in urine samples collected from 2004 to 2018. However, a significantly higher 8-carboxygeraniol excretion per 24 h was observed in females compared to males across the sampling years from 2004 to 2012. This trend equalized in the years 2015 and 2018. We could demonstrate that 8-carboxygeraniol may be a suited biomarker for assessing the geraniol exposure in the general population. Regardless of the fact that additional, preferably population representative studies combining HBM and health examination were helpful to further elucidate the risks of a geraniol exposure, the current study adds important data for identifying time trends and body burden of geraniol in the environment and shows the ubiquitous exposure towards mixtures of sensitizing chemicals. doi: 10.1016/j.ijheh.2021.113880
Lessmann, Frederik; Kolossa-Gehring, Marike; Apel, Petra; Rüther, Maria; Pälmke, Claudia; Harth, Volker; Brüning, Thomas; Koch, Holger Martin Environment International 132 (2019), 105102 The worldwide plasticizer markets are facing constant substitution processes. Many classic ortho-phthalate plasticizers like di(2-ethylhexyl) phthalate (DEHP) are phased out, due to their proven toxicity to reproduction. Assumedly less critical, less regulated plasticizers such as di(2-ethylhexyl) terephthalate (DEHTP) are increasingly applied in consumer near products like toys, food contact materials, and medical devices. With the increasing use of DEHTP, increasing exposures of the general population have to be expected likewise. Human biomonitoring is a well-established tool to determine population exposures. In the present study we investigate the time trend of exposure to DEHTP using 24-hour urine samples of the German Environmental Specimen Bank (ESB) collected from 1999 to 2017. In these samples (60 per odd-numbered year, 600 samples in total) collected from young German adults (20-29 years, equal gender distribution) we determined four specific urinary me-tabolites as biomarkers of DEHTP exposure. From 1999 to 2009, the main specific urinary metabolite 5cx-MEPTP was quantifiable in < 10% of the samples. Thereafter, detection rates and levels constantly increased, in line with rapidly increasing DEHTP consumption volumes. In 2017, all samples had 5cx-MEPTP levels above the limit of quantification (LOQ) with a median concentration of 3.35 μg/L (95th percentile: 12.8 μg/L). The other metabolites were detected less frequently and at lower levels but correlated well with 5cx-MEPTP robustly confirming the increasing DEHTP exposure. All 5cx-MEPTP concentrations were well below the German health based guidance value (HBM-I) of 2800 μg/L for adults. Likewise, the median calculated daily intake, based on 5cx-MEPTP measured in 2017, was 0.74 μg/kg bw * d (95th percentile: 3.86 μg/kg bw * d), still well below the tolerable daily intake (TDI) of 1000 μg/kg bw * d. Based on current toxicological knowledge we can hence conclude that for the population investigated, DEHTP exposure gives no reason for immediate concern. However, the steep ongoing increase of DEHTP exposure warrants further close monitoring in the future, preferably also in sub-populations with known higher exposures to plasticizers, especially children. doi: 10.1016/j.envint.2019.105102
Schettgen, Thomas; Bertram, Jens; Kraus, Thomas; Kolossa-Gehring, Marike Analytical Methods 13 (2021), 1847-1856; online 16. März 2021 Methylisothiazolinone and the reaction mixture of chloromethylisothiazolinone/methylisothiazolinone (MCI/MI, 3 : 1) are broadly used biocides that are contained in many products of everyday life (e.g. cosmetics, wet wipes, etc.). As MI and MCI are able to sensitize (and penetrate) the skin, their application in cosmetic products is of concern. In previous work, we have revealed a background exposure of the general population to MI and/or MCI/MI (3 : 1) by the determination of urinary N-methylmalonamic acid (NMMA) as the main human metabolite. To corroborate these findings, we have now developed a two-dimensional LC/MS/MS method for the quantification of a mercapturic acid metabolite of MI and MCI ((acetylamino){[3-(methylamino)-1-(methylthio)-3-oxopropyl]thio}acetic acid or shortly “M-12”) in human urine. This analyte is enriched online using a Strata-X-column and stripped from the urinary matrix. Then, the analyte is back flushed to the analytical column (Phenomenex C18(2), 150 × 4.6 mm) and finally quantified by tandem mass spectrometry with the use of isotopically labelled M-12 as the internal standard. The LOQ for M-12 was 0.2 ng mL−1 urine and sufficient to quantify urinary background levels. Precision within and between series for M-12 in urine at concentrations varying from 0.2 to 5 ng mL−1 ranged from 2.1 to 23.9% and accuracy ranged from 86.3 to 101.8%. Mean accuracy for M-12 in individual urine samples was 94.3% (range: 89.7–102.9%). We applied this method to previously collected 24 h urine samples of 60 persons with no specific exposure to MI and/or MCI/MI (3 : 1). The metabolite M-12 could be quantified in each urine sample. The median and 95th percentile levels for urinary M-12 were determined to be 0.62 and 2.26 ng mL−1, respectively. In these urine samples, the concentrations of the previously determined metabolite NMMA and M-12 correlated well. In the future, we will apply this method to urine samples of a previously conducted human exposure study to explore the additional value of M-12 as a biomarker of exposure to MI and MCI. doi: 10.1039/d1ay00183c
Kolossa-Gehring, Marike; Becker, Kerstin; Conrad, André; Schröter-Kermani, Christa; Schulz, Christine; Seiwert, Margarete In: Knudsen, Lisbeth; Merlo, Domenico F. (Eds): Biomarkers and Human Biomonitoring Volume 1: Ongoing Programs and Exposures, RSC Publishing, Cambridge, UK (2012), 16-45 The German human biomonitoring system on a national level consists of two main instruments: the German Environmental Survey and the Environmental Specimen Bank. The German Environmental Survey (GerES) is a nationwide population study which has been carried out repeatedly in Germany since the mid-1980s. Human biomonitoring data are representative for people living in Germany with regard to age, gender and community size. The GerES I for adults was carried out in 1985/1986 (West Germany), followed by GerES IIa in 1990/91 (West Germany) and GerES IIb in 1991/92 (East Germany). In GerES II, the children of participating parents were also included. In 1998, GerES III for adults was conducted in the reunified Germany. GerES IV (2003/2006) focused exclusively on children. To elucidate exposure pathways and thus support the development of measures to reduce exposure, GerES uses three main instruments: human biomonitoring, ambient monitoring, and questionnaires. GerES I–IV have been conducted in close co-operation with the concurrent National Health Interview and Examination Surveys performed by the Robert Koch Institute, Berlin. The Environmental Specimen Bank (ESB) started routine operation in 1985. Human specimens are taken annually from students at four German university towns, archived as individual samples, and stored at temperatures below –150 °C. After more than two decades of operation the ESB now provides a continuous historical record of the state of exposure of humans and the environment in Germany for this period, thus supplying samples for retrospective monitoring of emerging pollutants, and the identification of temporal trends and spatial load differences. doi:10.1039/9781849733373-00016
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