Person: Murawski, Aline
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Veröffentlichung Alkyl pyrrolidone solvents N-methyl-2-pyrrolidone (NMP) and N-ethyl-2-pyrrolidone (NEP) in urine of children and adolescents in Germany - human biomonitoring results of the German Environmental Survey 2014-2017 (GerES V)(2021) Kolossa-Gehring, Marike; Murawski, Aline; Rucic, Enrico; Schmied-Tobies, Maria Irene Hilde; Schwedler, GerdaN-methyl-2-pyrrolidone (NMP) and its substitute N-ethyl-2-pyrrolidone (NEP) are aprotic solvents used in many technical applications, but also in carpets, and consumer products such as cleaning agents, and cosmetics. NMP and NEP are classified as reproductive toxicants. As a substance of very high concern (SVHC), NMP is included in the European REACH (Registration, Evaluation, Authorisation of Chemicals) candidate list for authorisation. NMP and NEP metabolites were measured in more than 2100 urine samples of 3- to 17-year-old children and adolescents, participating in the population-representative German Environmental Survey for Children and Adolescents 2014-2017 (GerES V). The two NMP metabolites 5-hydroxy-N-methyl-2-pyrrolidone (5-HNMP) and 2-hydroxy-N-methylsuccinimide (2-HMSI) could be detected and quantified in all urine samples, and the two NEP metabolites 5-hydroxy-N-ethylpyrrolidone (5-HNEP) and 2-hydroxy-N-ethylsuccinimide (2-HESI) in 32% and 87% of the urine samples. Geometric mean concentrations were 103.1 (my)g/L (88.21 (my)g/gcreatinine) for the sum of NMP metabolites and 11.86 Ìg/L (10.15 (my)g/gcreatinine) for the sum of NEP metabolites, thus remaining below the current health-based human biomonitoring values. For NMP, highest exposure was found in young children, but exposure pathways could not be revealed. Exposure to NEP was highest in adolescents and participants with low socio-economic status or migration background. Associations to usage of personal care products suggested the choice of products to have a distinct impact on NEP exposure. The presented data can be used by the German Human Biomonitoring Commission to derive new reference values (RV95) for NMP and NEP for children and adolescents in Germany. This will facilitate to recognise changing exposure levels in this population group in Germany. © 2020 The Author(s).Veröffentlichung Determination of trace elements in urine by inductively coupled plasma-tandem mass spectrometry - Biomonitoring of adults in the German capital region(2021) Schmied, Andy; Kolossa-Gehring, Marike; Murawski, AlineA method was developed and validated for multi-element analyses of human urine samples using inductively coupled plasma-tandem mass spectrometry. The combination of a simple sample preparation and the state-of-the-art technique allows high-throughput and lowest limits of quantification up to 1 ng/L. Thereby coefficients of variation ranges from 0.4% (V) to 3.7% (Be), and 0.9% (Cd) to 4.8% (Ni) for intraday and interday precision, respectively. The method's performance is demonstrated by successful participation in international interlaboratory comparison programs as external quality assurance. Moreover, the method was applied for the analysis of first-morning void urine samples of adults (N = 77) living in the German capital region. 15 metals and metalloids (Astotal, Be, Bi, Cd, Co, Cr, In, Mn, Mo, Ni, Pb, Sn, Tl, V, and Zn) were determined. With exception of indium, all elements were found in urine samples above the limit of quantification, demonstrating the suitability to measure the general population's exposure to these metals and metalloids. The method presented here shall be used for analysis of urine samples collected in the upcoming German Environmental Survey, GerES VI, a cross-sectional, population-representative study. Quelle: © Elsevier 2021Veröffentlichung Substitutes mimic the exposure behaviour of REACH regulated phthalates(2021) Apel, Petra; Kolossa-Gehring, Marike; Lange, Rosa; Lemke, Nora; Debiak, Malgorzata; Murawski, Aline; Weber, TillThe population is constantly exposed to potentially harmful substances present in the environment, including inter alia food and drinking water, consumer products, and indoor air. Human biomonitoring (HBM) is a valuable tool to determine the integral, internal exposure of the general population, including vulnerable subgroups, to provide the basis for risk assessment and policy advice. The German HBM system comprises of five pillars: (1) the development of suitable analytical methods for new substances of concern, (2) cross-sectional population-representative German Environmental Surveys (GerES), (3) time trend analyses using archived samples from the Environmental Specimen Bank (ESB), (4) the derivation of health-based guidance values as a risk assessment tool, and (5) transfer of data into the European cooperation network HBM4EU. The goal of this paper is to present the complementary elements of the German HBM system and to show its strengths and limitations on the example of plasticizers. Plasticizers have been identified by EU services and HBM4EU partners as priority substances for chemical policy at EU level. Using the complementary elements of the German HBM system, the internal exposure to classical phthalates and novel alternative plasticizers can be reliably monitored. It is shown that market changes, due to regulation of certain phthalates and the rise of substitutes, are rapidly reflected in the internal exposure of the population. It was shown that exposure to DEHP, DiBP, DnBP, and BBzP decreased considerably, whereas exposure to the novel substitutes such as DPHP, DEHTP, and Hexamoll®DINCH has increased significantly. While health-based guidance values for several phthalates (esp. DnBP, DiBP, DEHP) were exceeded quite often at the turn of the millennium, exceedances today have become rarer. Still, also the latest GerES reveals the ubiquitous and concurrent exposures to many plasticizers. Of concern is that the youngest children showed the highest exposures to most of the investigated plasticizers and in some cases their levels of DiBP and DnBP still exceeded health-based guidance values. Over the last years, mixture exposures are increasingly recognized as relevant, especially if the toxicological modes of action are similar. This is supported by a cumulative risk assessment for four endocrine active phthalates which confirms the still concerning cumulative exposure in many young children. Given the adverse health effects of some phthalates and the limited toxicological knowledge of substitutes, exposure reduction and surveillance are needed on German and EU-level. Substitutes need to be monitored, to intervene if exposures are threatening to exceed acceptable levels, or if new toxicological data question their appropriateness. It is strongly recommended to reconsider the use of plastics and plasticizers. © 2021 Published by Elsevier GmbH.Veröffentlichung 2-Mercaptobenzothiazole in urine of children and adolescents in Germany - Human biomonitoring results of the German Environmental Survey 2014-2017 (GerES V)(2020) Conrad, André; Kolossa-Gehring, Marike; Murawski, Aline; Rucic, Enrico; Schmied-Tobies, Maria Irene Hilde; Schwedler, Gerda2-Mercaptobenzothiazole (2-MBT) is widely used as a vulcanisation accelerator and is contained in many products made from natural rubber, e.g. car tires. Additionally, it is used as a fungicide in paint or fibre. Systemically human exposure to 2-MBT can occur via dermal and oral uptake or inhalation. Locally, 2-MBT can cause skin sensitisation. The International Agency for Research on Cancer (IARC) classified 2-MBT as probably carcinogenic to humans. 516 urine samples of 3- to 17-year-old children and adolescents living in Germany were analysed for the concentration of 2-MBT in the population representative German Environmental Survey for Children and Adolescents 2014-2017 (GerES V). 2-MBT was quantified above the limit of quantification (LOQ) of 1.0 my g/L in 50% of the 516 samples analysed. The geometric mean of urinary 2-MBT concentration was 1.018 my g/L and 0.892 my g/gcreatinine, the arithmetic mean was 1.576 my g/L (1.351 myg/gcrea). The median concentration was below the LOQ. Analyses of subgroups revealed higher 2-MBT concentrations in children aged 3-5 years compared to 14- to 17-year-old adolescents. All urinary 2-MBT concentrations were well below the health-based guidance value HBM-I for children of 4.5 my g/L. Therefore, current exposure levels are - according to current knowledge - not of concern. For the first time, reference values can be derived for 2-MBT for children and adolescents in Germany. This will facilitate to recognise changing exposure levels in this population group in Germany and identification of unusually high exposures. © 2020 The Authors.Veröffentlichung Deutsche Umweltstudie zur Gesundheit von Kindern und Jugendlichen 2014-2017 (GerES V)(Umweltbundesamt, 2023) Hahn, Domenica; Kolossa-Gehring, Marike; Lange, Rosa; Lemke, Nora; Murawski, Aline; Peisker, Jasmin; Debiak, Malgorzata; Rucic, Enrico; Zimmermann, Philipp; David, Madlen; Gerofke, Antje; Weber, Till; Pack, Kim LauraIn der Deutschen Umweltstudie zur Gesundheit (GerES) wird die Schadstoff-Belastung der Bevölkerung repräsentativ für die Menschen in Deutschland erhoben. In der fünften Erhebung, GerESV (2014-2017), wurden 2.294 Kinder und Jugendliche im Alter von 3 bis 17 Jahren aus 167 Orten in ganz Deutschland untersucht. GerES V ist eine bevölkerungsrepräsentative Querschnittstudie und wurde in enger Kooperation mit der "Studie zur Gesundheit von Kindern und Jugendlichen in Deutschland" (KiGGS Welle 2) des Robert-Koch-Instituts durchgeführt. Im Human-Biomonitoring (HBM) von GerESV wurden 107 verschiedene Substanzen im Blut bzw. Urin der Teilnehmenden gemessen. Der vorliegende Bericht fasst die HBM-Ergebnisse von GerESV zusammen. Bei Vorliegen entsprechender Beurteilungswerte wird eine gesundheitliche Bewertung vorgenommen. Der Bericht gibt einen Überblick über die Abläufe der Datenerhebung und die chemisch-analytischen und statistischen Methoden. Die wichtigsten Ergebnisse zu Belastungsquellen und -pfaden sowie besonders belasteten Bevölkerungsgruppen sind zusammengefasst und in aggregierter Form tabellarisch präsentiert. Für jede untersuchte Substanz werden außerdem die Quellen, die toxikologischen Eigenschaften und aktuellen Regulationen aufgeführt. Die bisherige Nutzung der Daten aus GerES V für Politik- und Öffentlichkeitsarbeit sowie in internationalen Kooperationen ist ebenfalls dargelegt. Quelle: ForschungsberichtVeröffentlichung Exposure to phthalates in European children, adolescents and adults since 2005: a harmonized approach based on existing HBM data in the HBM4EU Initiative(2023) Kolossa-Gehring, Marike; Lange, Rosa; Murawski, Aline; Rüther, Maria; Gerofke, Antje; Schmidt, Phillipp; Springer, Andrea; Vogel, Nina; Weber, TillPhthalates are mainly used as plasticizers and are associated inter alia with adverse effects on reproductive functions. While more and more national programs in Europe have started monitoring internal exposure to phthalates and its substitute 1,2-Cyclohexanedicarboxylic acid (DINCH), the comparability of results from such existing human biomonitoring (HBM) studies across Europe is challenging. They differ widely in time periods, study samples, degree of geographical coverage, design, analytical methodology, biomarker selection, and analytical quality assurance level. The HBM4EU initiative has gathered existing HBM data of 29 studies from participating countries, covering all European regions and Israel. The data were prepared and aggregated by a harmonized procedure with the aim to describe - as comparably as possible - the EU-wide general population's internal exposure to phthalates from the years 2005 to 2019. Most data were available from Northern (up to 6 studies and up to 13 time points), Western (11; 19), and Eastern Europe (9; 12), e.g., allowing for the investigation of time patterns. While the bandwidth of exposure was generally similar, we still observed regional differences for Butyl benzyl phthalate (BBzP), Di(2-ethylhexyl) phthalate (DEHP), Di-isononyl phthalate (DiNP), and Di-isobutyl phthalate (DiBP) with pronounced decreases over time in Northern and Western Europe, and to a lesser degree in Eastern Europe. Differences between age groups were visible for Di-n-butyl phthalate (DnBP), where children (3 to 5-year olds and 6 to 11-year olds) had lower urinary concentrations than adolescents (12 to 19-year-olds), who in turn had lower urinary concentrations than adults (20 to 39-year-olds). This study is a step towards making internal exposures to phthalates comparable across countries, although standardized data were not available, targeting European data sets harmonized with respect to data formatting and calculation of aggregated data (such as developed within HBM4EU), and highlights further suggestions for improved harmonization in future studies. © 2023 by the authorsVeröffentlichung Benzene metabolite SPMA and acrylamide metabolites AAMA and GAMA in urine of children and adolescents in Germany - human biomonitoring results of the German Environmental Survey 2014-2017 (GerES V)(2020) Bethke, Robert; Kolossa-Gehring, Marike; Murawski, Aline; Rucic, Enrico; Schmied-Tobies, Maria Irene Hilde; Schwedler, GerdaBenzene and acrylamide are carcinogenic substances contained inter alia in tobacco smoke. The mercapturic acid metabolites of benzene, N-acetyl-S-phenyl-L-cysteine (SPMA), and of acrylamide, N-acetyl-S-(3-amino-3-oxopropyl)-cysteine (AAMA) and N-acetyl-S-(3-amino-2-hydroxy-3-oxopropyl)-cysteine (GAMA), were analysed in 2260 first-morning void urine samples from children and adolescents aged 3-17 years, participating in the population-representative German Environmental Survey on Children and Adolescents, GerES V 2014-2017. SPMA was detected in 98% of the participants with a geometric mean (GM) of 0.097 (my)g/L urine. Smokers had about 10-fold higher levels of the benzene metabolite SPMA than non-smokers. The sample comprises of 48 self-reported smokers, mainly in the oldest age group (14-17-year-olds). Second-hand smoke exposure, living near busy or very busy roads, and using domestic fuels for heating were additionally associated with higher benzene metabolite levels. SPMA levels in GerES V were lower compared to levels found in other countries, which in part however may reflect different proportions of smokers. The acrylamide metabolites AAMA and GAMA were detected in 100% of the participants with a GM of 72.6 (my)g/L urine for AAMA and 15.0 (my)g/L urine for GAMA. Smoking children and adolescents had about 2.5-fold higher AAMA levels than non-smoking ones. The frequency of consumption of french-fried potatoes and potato crisps consumption was also positively associated with urinary AAMA and GAMA levels. Compared to the urinary AAMA and GAMA levels in Germany and other countries, levels in GerES V tended to be higher than in the few studies reported. The urinary levels of the benzene biomarker SPMA, and the acrylamide biomarkers AAMA and GAMA build the basis to derive reference values for the exposure of children and adolescents in Germany. The results reveal options for exposure reduction mainly in personal choices regarding smoking and diet, but also requiring policy to maintain efforts in non-smoking regulations and improving ambient air quality. Providing these results also to the European HBM Initiative HBM4EU will contribute to gain knowledge on the exposure of the European population, the health impact of carcinogens and thus providing support for substantiated exposure assessment. © 2020 The Author(s)Veröffentlichung Polychlorinated biphenyls (PCB) and organochlorine pesticides (OCP) in blood plasma - results of the German environmental survey for children and adolescents 2014-2017 (GerES V)(2020) Bandow, Nicole; Conrad, André; Kolossa-Gehring, Marike; Murawski, Aline; Sawal, GeorgeThe German Environmental Survey for Children and Adolescents 2014-2017 (GerES V) investigated the current internal exposure to polychlorinated biphenyls (PCB) and organochlorine pesticides (OCP). These analyses were carried out for a population-representative sub-sample of 1135 children and adolescents (aged 3-17 years) of all 2394 GerES V participants. Blood plasma samples were analyzed for seven indicator PCB (PCB 28, PCB 52, PCB 101, PCB 118, PCB 138, PCB 153 and PCB 180) and selected OCP (hexachlorobenzene, three hexachlorocyclohexane isomers, 4,4'-DDT, 4,4'-DDD and 4,4'-DDE). Despite risk mitigation measures and bans put into force some decades ago children and adolescents living in Germany are still exposed to PCB and OCP: Highest geometric mean plasma concentrations were measured for 4,4'-DDE (0.158 g/L), followed by PCB 138 (0.049 g/L), PCB 153 (0.066 g/L) and PCB 180 (0.032 g/L). Different application patterns of compounds between former East and former West Germany are still reflected by differences in plasma concentrations. Significant differences between age groups and by sexes were found. Moreover, the influence of breastfeeding and fish consumption, which was also found in other studies, was confirmed. Comparison with the results of GerES 2003-2006 confirms a decreasing trend in blood samples observed world-wide. Currently, health-based guidance values for PCB are still exceeded, though to a very limited extent. Also, the widespread occurrence of these compounds underlines the need for further monitoring of these compounds in humans although they are no longer marketed. Quelle: https://www.sciencedirect.comVeröffentlichung Harmonized human biomonitoring in European children, teenagers and adults: EU-wide exposure data of 11 chemical substance groups from the HBM4EU Aligned Studies (2014-2021)(2023) Govarts, Eva; Apel, Petra; Gilles, Liese; Rodriguez Martin, Laura; Kolossa-Gehring, Marike; Lange, Rosa; Lemke, Nora; Murawski, Aline; Rüther, Maria; Vogel, Nina; Weber, Till; Zimmermann, PhilippAs one of the core elements of the European Human Biomonitoring Initiative (HBM4EU) a human biomonitoring (HBM) survey was conducted in 23 countries to generate EU-wide comparable HBM data. This survey has built on existing HBM capacity in Europe by aligning national or regional HBM studies, referred to as the HBM4EU Aligned Studies. The HBM4EU Aligned Studies included a total of 10,795 participants of three age groups: (i) 3,576 children aged 6-12 years, (ii) 3,117 teenagers aged 12-18 years and (iii) 4,102 young adults aged 20-39 years. The participants were recruited between 2014 and 2021 in 11-12 countries per age group, geographically distributed across Europe. Depending on the age group, internal exposure to phthalates and the substitute DINCH, halogenated and organophosphorus flame retardants, per- and polyfluoroalkyl substances (PFASs), cadmium, bisphenols, polycyclic aromatic hydrocarbons (PAHs), arsenic species, acrylamide, mycotoxins (deoxynivalenol (total DON)), benzophenones and selected pesticides was assessed by measuring substance specific biomarkers subjected to stringent quality control programs for chemical analysis. For substance groups analyzed in different age groups higher average exposure levels were observed in the youngest age group, i.e., phthalates/DINCH in children versus teenagers, acrylamide and pesticides in children versus adults, benzophenones in teenagers versus adults. Many biomarkers in teenagers and adults varied significantly according to educational attainment, with higher exposure levels of bisphenols, phthalates, benzophenones, PAHs and acrylamide in participants (from households) with lower educational attainment, while teenagers from households with higher educational attainment have higher exposure levels for PFASs and arsenic. In children, a social gradient was only observed for the non-specific pyrethroid metabolite 3-PBA and di-isodecyl phthalate (DiDP), with higher levels in children from households with higher educational attainment. Geographical variations were seen for all exposure biomarkers. For 15 biomarkers, the available health-based HBM guidance values were exceeded with highest exceedance rates for toxicologically relevant arsenic in teenagers (40%), 3-PBA in children (36%), and between 11 and 14% for total DON, Summe (PFOA + PFNA + PFHxS + PFOS), bisphenol S and cadmium. The infrastructure and harmonized approach succeeded in obtaining comparable European wide internal exposure data for a prioritized set of 11 chemical groups. These data serve as a reference for comparison at the global level, provide a baseline to compare the efficacy of the European Commission's chemical strategy for sustainability and will give leverage to national policy makers for the implementation of targeted measures. © 2023 The AuthorsVeröffentlichung Current exposure to phthalates and DINCH in European children and adolescents - results from the HBM4EU Aligned Studies 2014 to 2021(2023) Kolossa-Gehring, Marike; Lange, Rosa; Gerofke, Antje; Murawski, Aline; Schmidt, Phillipp; Vogel, NinaPhthalates are mainly used as plasticizers for polyvinyl chloride (PVC). Exposure to several phthalates is associated with different adverse effects most prominently on the development of reproductive functions. The HBM4EU Aligned Studies (2014-2021) have investigated current European exposure to ten phthalates (DEP, BBzP, DiBP, DnBP, DCHP, DnPeP, DEHP, DiNP, DiDP, DnOP) and the substitute DINCH to answer the open policy relevant questions which were defined by HBM4EU partner countries and EU institutions as the starting point of the programme. The exposure dataset includes ~5,600 children (6-11 years) and adolescents (12-18 years) from up to 12 countries per age group and covering the North, East, South and West European regions. Study data from participating studies were harmonised with respect to sample size and selection of participants, selection of biomarkers, and quality and comparability of analytical results to provide a comparable perspective of European exposure. Phthalate and DINCH exposure were deduced from urinary excretions of metabolites, where concentrations were expressed as their key descriptor geometric mean (GM) and 95th percentile (P95). This study aims at reporting current exposure levels and differences in these between European studies and regions, as well as comparisons to human biomonitoring guidance values (HBM-GVs). GMs for children were highest for total-DEHP metabolites (33.6 mikrog/L), MiBP (26.6 mikrog/L), and MEP (24.4 mikrog/L) and lowest for total-DiDP metabolites (1.91 mikrog/L) and total-DINCH metabolites (3.57 mikrog/L). In adolescents highest GMs were found for MEP (43.3 mikrog/L), total-DEHP metabolites (28.8 mikrog/L), and MiBP (25.6 mikrog/L) and lowest for total-DiDP metabolites (= 2.02 mikrog/L) and total-DINCH metabolites (2.51 mikrog/L). In addition, GMs and P95 stratified by European region, sex, household education level, and degree of urbanization are presented. Differences in average biomarker concentrations between sampling sites (data collections) ranged from factor 2 to 9. Compared to the European average, children in the sampling sites OCC (Denmark), InAirQ (Hungary), and SPECIMEn (The Netherlands) had the lowest concentrations across all metabolites and ESTEBAN (France), NAC II (Italy), and CROME (Greece) the highest. For adolescents, comparably higher metabolite concentrations were found in NEB II (Norway), PCB cohort (Slovakia), and ESTEBAN (France), and lower concentrations in POLAES (Poland), FLEHS IV (Belgium), and GerES V-sub (Germany). Multivariate analyses (Survey Generalized Linear Models) indicate compound-specific differences in average metabolite concentrations between the four European regions. Comparison of individual levels with HBM-GVs revealed highest rates of exceedances for DnBP and DiBP, with up to 3 and 5%, respectively, in children and adolescents. No exceedances were observed for DEP and DINCH. With our results we provide current, detailed, and comparable data on exposure to phthalates in children and - for the first time - in adolescents, and - for the first time - on DINCH in children and adolescents of all four regions of Europe which are particularly suited to inform exposure and risk assessment and answer open policy relevant questions. © 2023 The Authors.