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Veröffentlichung Phthalate metabolites in 24-h urine samples of the German Environmental Specimen Bank (ESB) from 1988 to 2015 and a comparison with US NHANES data from 1999 to 2012(2017) Koch, Holger M.; Apel, Petra; Schütze, Andre; Conrad, André; Pälmke, Claudia; Kolossa-Gehring, Marike; Brüning, Thomas; Rüther, MariaThe German Environmental Specimen Bank (ESB) continuously collects 24-h urine samples since theearly 1980s in Germany. In this study we analyzed 300 urine samples from the years 2007 to 2015 for 21phthalate metabolites (representing exposure to 11 parent phthalates) and combined the data with twoprevious retrospective measurement campaigns (1988 to 2003 and 2002 to 2008). The combined datasetcomprised 1162 24-h urine samples spanning the years 1988 to 2015. With this detailed set of humanbiomonitoring data we describe the time course of phthalate exposure in Germany over a time frame of27 years. For the metabolites of the endocrine disrupting phthalates di(2-ethylhexyl) phthalate (DEHP),di-n-butyl phthalate (DnBP) and butylbenzyl phthalate (BBzP) we observed a roughly ten-fold decline inmedian metabolite levels from their peak levels in the late 1980s/early 1990s compared to most recentlevels from 2015. Probably, bans (first enacted in 1999) and classifications/labelings (enacted in 2001 and2004) in the European Union lead to this drop. A decline in di-isobutyl phthalate (DiBP) metabolite levelsset in only quite recently, possibly due to its later classification as a reproductive toxicant in the EU in 2009.In a considerable number of samples collected before 2002 health based guidance values (BE, HBM I) havebeen exceeded for DnBP (27.2%) and DEHP (2.3%) but also in recent samples some individual exceedancescan still be observed (DEHP 1.0%). A decrease in concentration for all low molecular weight phthalates,labelled or not, was seen in the most recent years of sampling. For the high molecular weight phthalates,DEHP seems to have been substituted in part by di-isononyl phthalate (DiNP), but DiNP metabolite levelshave also been declining in the last years. Probably, non-phthalate alternatives increasingly take overfor the phthalates in Germany. A comparison with NHANES (National Health and Nutrition ExaminationSurvey) data from the United States covering the years 1999 to 2012 revealed both similarities anddifferences in phthalate exposure between Germany and the US. Exposure to critical phthalates hasdecreased in both countries with metabolite levels more and more aligning with each other, but highmolecular weight phthalates substituting DEHP (such as DiNP) seem to become more important in theUS than in Germany.
© 2016 Elsevier GmbH. All rights reservedVeröffentlichung Urinary phthalate concentrations in mothers and their children in Ireland(2017) Cullen, Elizabeth; Evans, David; Griffin, Chris; Kolossa-Gehring, Marike; Schwedler, GerdaVeröffentlichung Advancing human health risk assessment(2019) Lanzoni, Anna; Castoldi, Anna F.; Kass, George EN; Kolossa-Gehring, MarikeThe current/traditional human health risk assessment paradigm is challenged by recent scientific and technical advances, and ethical demands. The current approach is considered too resource intensive, is not always reliable, can raise issues of reproducibility, is mostly animal based and does not necessarily provide an understanding of the underlying mechanisms of toxicity. From an ethical and scientific viewpoint, a paradigm shift is required to deliver testing strategies that enable reliable, animal-free hazard and risk assessments, which are based on a mechanistic understanding of chemical toxicity and make use of exposure science and epidemiological data. This shift will require a new philosophy, new data, multidisciplinary expertise and more flexible regulations. Re-engineering of available data is also deemed necessary as data should be accessible, readable, interpretable and usable. Dedicated training to build the capacity in terms of expertise is necessary, together with practical resources allocated to education. The dialogue between risk assessors, risk managers, academia and stakeholders should be promoted further to understand scientific and societal needs. Genuine interest in taking risk assessment forward should drive the change and should be supported by flexible funding. This publication builds upon presentations made and discussions held during the break-out session 'Advancing risk assessment science - Human health' at EFSA's third Scientific Conference 'Science, Food and Society' (Parma, Italy, 18ââą Ì21 September 2018). © 2019 European Food Safety AuthorityVeröffentlichung Polycyclic aromatic hydrocarbons (PAH) 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; Roth, Alexandra; Rucic, Enrico; Schmied-Tobies, Maria Irene Hilde; Schwedler, GerdaPolycyclic aromatic hydrocarbons (PAH) mainly originate from incomplete combustion of organic materials and are, among other sources, found in traffic emissions, smoked or barbecued food, leafy vegetables, and tobacco smoke. Some PAH or their metabolites are hazardous for health and classified as carcinogenic, mutagenic, or toxic to reproduction. Urine samples from 3- to 17-year-old children and adolescents living in Germany were analysed for concentrations of metabolites of the PAH fluorene, naphthalene, phenanthrene, and pyrene in the population-representative German Environmental Survey for Children and Adolescents GerES V (2014-2017). PAH metabolites were analysed in urine samples of 516 participants and could be quantified in 88ââą Ì100% of the samples. Geometric mean concentrations were: 0.785 my g/L (0.688 my g/gcreatinine) for 1-OH-naphthalene, 4.233 my g/L (3.706 my g/gcrea) for 2-OH-naphthalene, 0.139 my g/L (0.122 my g/gcrea) for 1-OH-phenanthrene, 0.085 my g/L (0.075 my g/gcrea) for 2-OH-phenanthrene, 0.131 my g/L (0.115 my g/gcrea) for 3-OH-phenanthrene, 0.045 my g/L (0.040 my g/gcrea) for 4-OH-phenanthrene, 0.058 my g/L (0.050 my g/gcrea) for 9-OH-phenanthrene, 0.511 my g/L (0.448 my g/gcrea) for Σ-OH-phenanthrene, and 0.099 my/L (0.087 my g/gcrea) for 1-OH-pyrene. Analyses of subgroups revealed higher PAH metabolite concentrations in young children compared to adolescents, and also in residents of former East Germany compared to those living in former West Germany. Increased urinary PAH metabolite concentrations were found in participants using domestic fuel for heating or gas for cooking. Plastic objects were identified as another potential source of exposure. Urinary concentrations of naphthalene and fluorene metabolites were elevated in active smokers and to the same extent in non-smokers exposed to passive smoking. Comparison with previous cycles of GerES revealed a decrease over time and a further decline in the still significant differences in urinary PAH metabolite concentrations of participants living in former East versus West Germany. © 2020 Published by Elsevier GmbH.Veröffentlichung Phthalate metabolites in urine of children and adolescents in Germany. Human biomonitoring results of the German Environmental Survey GerES V, 2014-2017(2020) Conrad, André; Daniels, Anja; Kolossa-Gehring, Marike; Lange, Rosa; Rucic, Enrico; Schmied-Tobies, Maria Irene Hilde; Schulz, Christine; Schwedler, GerdaDuring the population representative German Environmental Survey of Children and Adolescents (GerES V, 2014-2017) 2256 first-morning void urine samples from 3 to 17 years old children and adolescents were analysed for 21 metabolites of 11 different phthalates (di-methyl phthalate (DMP), di-ethyl phthalate (DEP), butylbenzyl phthalate (BBzP), di-iso-butyl phthalate (DiBP), di-n-butyl phthalate (DnBP), di-cyclohexyl phthalate (DCHP), di-n-pentyl phthalate (DnPeP), di-(2-ethylhexyl) phthalate (DEHP), di-iso-nonyl phthalate (DiNP), di-iso-decyl phthalate (DiDP) and di-n-octyl phthalate (DnOP)). Metabolites of DMP, DEP, BBzP, DiBP, DnBP, DEHP, DiNP and DiDP were found in 97-100% of the participants, DCHP and DnPeP in 6%, and DnOP in none of the urine samples. Geometric means (GM) were highest for metabolites of DiBP (MiBP: 26.1 my g/L), DEP (MEP: 25.8 my g/L), DnBP (MnBP: 20.9 my g/L), and DEHP (cx-MEPP: 11.9 my g/L). For all phthalates but DEP, GMs were consistently higher in the 3-5 years old children than in the 14-17 years old adolescents. For DEHP, the age differences were most pronounced. All detectable phthalate biomarker concentrations were positively associated with the levels of the respective phthalate in house dust. In GerES V we found considerably lower phthalate biomarker levels than in the preceding GerES IV (2003-2006). GMs of biomarker levels in GerES V were only 18% (BBzP), 23% (MnBP), 23% (DEHP), 29% (MiBP) and 57% (DiNP) of those measured a decade earlier in GerES IV. However, some children and adolescents still exceeded health-based guidance values in the current GerES V. 0.38% of the participants had levels of DnBP, 0.08% levels of DEHP and 0.007% levels of DiNP which were higher than the respective health-based guidance values. Accordingly, for these persons an impact on health cannot be excluded with sufficient certainty. The ongoing and substantial exposure of vulnerable children and adolescents to many phthalates confirms the need of a continued monitoring of established phthalates, whether regulated or not, as well as of potential substitutes. With this biomonitoring approach we provide a picture of current individual and cumulative exposure developments and body burdens to phthalates, thus providing support for timely and effective chemicals policies and legislation. © 2020 The Authors. 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 Metabolites of the fragrance 2-(4-tert-butylbenzyl)propionaldehyde (lysmeral) in urine of children and adolescents in Germany - Human biomonitoring results of the German Environmental Survey 2014-2017 (GerES V)(2020) Fiedler, Nina; Kolossa-Gehring, Marike; Murawski, Aline; Rucic, Enrico; Schmied-Tobies, Maria Irene Hilde; Schwedler, GerdaThe synthetic fragrance 2-(4-tert-butylbenzyl)propionaldehyde, also known as lysmeral, butylphenyl methylpropional, lilial, or lily aldehyde, is widely used in cosmetics, personal care products, laundry detergents, and air fresheners. It is classified as suspected to be harmful to fertility and possibly endocrine disrupting. Its maximum concentration in cosmetics is limited. First-morning void urine samples (N = 2133) were analysed for several metabolites of lysmeral (Chemical Abstract Service (CAS) No.: 80-54-6). Samples were collected in the population-representative German Environmental Survey for Children and Adolescents 2014-2017 (GerES V) from German residents aged 3-17 years. Four main metabolites tert-butylbenzoic acid, lysmerol, lysmerylic acid, and hydroxy-lysmerylic acid were found in quantifiable amounts in 100%, 99%, 40%, and 23% of the samples, respectively, with geometric mean concentrations of 10.21 my g/L (8.658 my g/gcrea) for tert-butylbenzoic acid, 1.528 my g/L (1.296 my g/gcrea) for lysmerol, and below the limit of quantification of 0.2 my g/L and 0.4 my g/L for lysmerylic acid and hydroxy-lysmerylic acid, respectively. Girls had higher urinary concentrations of lysmeral metabolites than boys. Usage of fragrances, fabric softener, and personal care products, especially perfume, was positively associated with urinary concentrations of lysmeral metabolites. Source identification builds a basis to derive proposals for reduction of exposure. These results can also provide the foundation for developing reference values for urinary metabolite concentrations of lysmeral in children and adolescents in Germany that will facilitate recognising future exposure trends. © 2020 The Author(s).Veröffentlichung Time trend of exposure to dechloranes: Plasma samples of German young adults from the environmental specimen bank collected from 1995 to 2017(2020) Fromme, Hermann; Thomsen, Cathrine; Aschenbrenner, Bettina; Kolossa-Gehring, Marike; Weber, TillDechloranes, like Dechlorane Plus® are commonly used flame retardants identified by the EU as substances of very high concern (SVHC) because of their persistence and bioaccumulation potential. To characterize the dechlorane exposure of Germans in the last two decades, 180 archived blood plasma samples of the German Environmental Specimen Bank (students aged 20-29 years) collected at six time points between 1995 and 2017 were analyzed for four dechloranes; namely Dechlorane Plus® (syn- and anti-DDC-CO), dechlorane 602 (DDC-DBF), and dechlorane 603 (DDC-Ant). These were quantified using a GC-MS/MS method. Overall, anti- and syn-DDC-CO were detected in 88% and 98% of the samples, whereas DDC-DBF and DDC-Ant were found in 40% and 37% of the samples, respectively. The median (95th percentile) values were 1.0 ng/g lipid weight (l.w.) (3.0 ng/g l.w.). for anti-DDC-CO, 0.6 ng/g l.w (1.9 ng/g l.w.). for syn-DDC-CO, 0.1 ng/g l.w (0.6 ng/g l.w.). for DDC-DBF, and 0.1 ng/g l.w (0.2 ng/g l.w.). for DDC-Ant. The 95th percentile concentrations of the sum of syn- and anti-DDC-CO decreased from 4.2 ng/g l.w. in 1995, to 2.9 ng/g l.w. in 1999, and subsequently increased to 3.7 ng/g l.w. in 2008, and up to 5.9 ng/g l.w. in 2017. A statistically significant decrease with time was observed for DDC-DBF and DDC-Ant, but not for DDC-CO. Our medians found in blood samples in 2017 are similar to those observed in Germany in 2013/14, but higher compared to values reported in other European countries. Overall, more toxicological and monitoring data is needed to better characterize the potential impact on health. © 2020 Elsevier GmbHVeröffentlichung 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 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).
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