Moos, Rebecca K.; Apel, Petra; Schröter-Kermani, Christa; Kolossa-Gehring, Marike; Brüning, Thomas; Koch, Holger M. Journal of Exposure Science and Environmental Epidemiology , online 30. November 2016 In recent years, exposure to parabens has become more of a concern because of evidence of ubiquitous exposure in the general population, combined with evidence of their potency as endocrine disruptors. New human metabolism data from oral exposure experiments enable us to back calculate daily paraben intakes from urinary paraben levels. We report daily intakes (DIs) for six parabens based on 660 24 h urine samples from the German Environmental Specimen Bank collected between 1995 and 2012. Median DI values ranged between 1.1 μg/kg bw/day for iso-butyl paraben and 47.5 μg/kg bw/day for methyl paraben. The calculated DIs were compared with acceptable levels of exposure to evaluate the hazard quotients (HQs) that indicate that acceptable exposure is exceeded for values of >1. Approximately 5% of our study population exceeded this threshold for individual paraben exposure. The hazard index (HI) that takes into account the cumulative risk of adverse estrogenic effects was 1.3 at the 95th percentile and 4.4 at maximum intakes, mainly driven by n-propyl paraben exposure. HI values of >1 indicate some level of concern. However, we have to point out that we applied most conservative assumptions in the HQ/HI calculations. Also, major exposure reduction measures were enacted in the European Union after 2012. doi:10.1038/jes.2016.65 Verwandte Publikation: Parabens in 24 h urine samples of the German Environmental Specimen Bank from 1995 to 2012
Schmidtkunz, Christoph; Küpper, Katja; Weber, Till; Leng, Gabriele; Kolossa-Gehring, Marike International Journal of Hygiene and Environmental Health 228 (2020), Juli 2020, 113541; online 5. Mai 2020 The antioxidant 2,6-di-tert-butyl-4-methylphenol (butylated hydroxytoluene, BHT) is used ubiquitously in food, cosmetics, pharmaceuticals, fuels, plastics, rubbers and many other products. Therefore, exposure of the general population to this substance is likely. We analyzed the BHT metabolite 3,5-di-tert-butyl-4-hydroxybenzoic acid (“BHT acid”) in 24-h urine samples from the German Environmental Specimen Bank with the aim of gaining a better understanding of the internal burden of BHT in young nonspecifically exposed adults. The study population consisted of students between 20 and 29 years of age at the time of sampling, all from Halle/Saale in Central Germany. In total, 329 samples collected in the years 2000, 2004, 2008, 2012, 2015, and 2018 were measured by ultra high performance liquid chromatography–tandem mass spectrometry (UHPLC-MS/MS). BHT acid was detected above the limit of quantification (0.2 μg/L) in 98% of the samples. The median of the measured concentrations was 1.06 μg/L and 1.24 μg/g creatinine respectively, the median of the daily excretion was 1.76 μg/24 h and – additionally normalized for body weight – 26.8 ng/24 h × kg bw respectively. The corresponding 90th percentiles were 3.28 μg/L, 3.91 μg/g creatinine, 5.05 μg/24 h, and 81.9 ng/24 h × kg bw. Medians of creatinine-corrected values were slightly higher in women than in men, while the opposite situation was observed for the volume concentrations and the 24-h excretion values (not corrected for body weight). Values simultaneously normalized both for 24-h excretion and body weight did not exhibit any significant differences between males and females, probably indicating a virtually identical magnitude of exposure for both genders. The background exposure of the investigated population was found to be largely constant since the year 2000, with only weak temporal trends at most. Daily intakes were estimated from excretion values and found to be largely below the acceptable daily intake (ADI) of BHT at 0.25 mg/kg bw: our worst-case estimate is a daily BHT intake of approximately 0.1 mg/kg bw at the 95th percentile level. However, these intake assessments rely on very limited quantitative data regarding human metabolism of BHT. doi: 10.1016/j.ijheh.2020.113541
Die gesundheitsschädigenden Wirkungen auf die Haut und die Augen des Menschen durch UV-Strahlung sind seit Jahren nachgewiesen und weiten Teilen der Bevölkerung bekannt. Der UV-B-Anteil der Sonnenstrahlung zieht bei Überdosierung als Akutreaktion den Sonnenbrand oder als chronischen Effekt eine Erhöhung des Hautkrebsrisikos nach sich. Derselbe UV-B-Bereich bewirkt aber auch die Einleitung der essentiellen Vitamin-D-Bildung. Die UV-induzierte Vitamin-D-Synthese in der Haut deckt zu mehr als 90 % den Vitamin-D-Bedarf ab, unsere typische Ernährung nur 10 %. Aufgrund dieser gegensätzlichen Wirkungen liegen widersprüchliche Empfehlungen in Bezug auf gesundheitsfördernde UV-Bestrahlung vor. Ziel des Vorhabens ist es, das quantitative sowie qualitative Verhältnis von UV-Exposition und Vitamin-D-Status im Körper unter verschiedenen Randbedingungen und in verschiedenen Bevölkerungsgruppen zu bestimmen. Hierauf basierend sollen Empfehlungen zur optimalen UV-Exposition differenziert nach Bevölkerungsgruppen erarbeitet werden, um den Ansprüchen an einen gesundheitsfördernden Strahlenschutz gerecht zu werden. Eine eingangs erstellte und abschließend aktualisierte Literaturstudie stellt den derzeitigen Kenntnisstand zum Vitamin-D-Stoffwechsel, zu den regulierenden Prozessen durch das Hormon Vitamin D3 und zum momentanen Diskussionsstand über den optimalen Vitamin-D-Status für den Menschen zusammen. In einer Serie von Studien wurde der Anstieg des Vitamin-D-Status (25OH-Vitamin D3 und 1,25OHVitamin D3) in Abhängigkeit von der UV-Exposition der Haut ermittelt. Expositionsparameter waren die biologisch wirksame UV-Dosis (bezogen auf die minimale Erythemdosis MED = persönliche Sonnenbrandschwellendosis der Probanden) und die Größe der bestrahlten Hautareale (zum einen alltagstypisch: Gesicht und Hände, zum anderen: der ganze Körper). Die seriellen UV-Expositionen erfolgten mit natürlicher solarer UV-Strahlung oder mit künstlicher simulierter Solarstrahlung oder mit Solarienstrahlung. Die insgesamt 240 Probanden wurden für die einzelnen Studien des Projektes bezüglich UV-Hauttyp II bzw. III, Alter und Geschlecht strukturiert rekrutiert. Erfasst wurden auch Daten bezüglich des Eigenschutzverhaltens der Haut gegenüber UV-Strahlung, um zu analysieren, inwieweit diese Faktoren einen Einfluss auf die Vitamin-D-Bildungseffizienz haben. FAZIT: In den Wintermonaten, vor Beginn der jeweiligen Untersuchungen, lag der Mittelwert für das 25OHVitamin D3 mit 18 ng/ml unterhalb des Normbereiches (20-60 ng/ml). Zweimal wöchentliche UV-Expositionen mit 10 % der MED senkrecht auf Gesicht und Hände bewirkten einen signifikanten Anstieg des Vitamin-D-Status. Der Zuwachs stieg mit der UV-Dosis und/oder mit der bestrahlten Körperfläche bei UV-Strahlung, die der Mittagssommersonne entspricht. Die Expositionen mit simulierter Solarstrahlung führten unter identischen Bedingungen (auch klimatisch) zu gleichen 25OHD-Anstiegen unabhängig von Ausgangsstatus. Bei den Solarexpositionen traten deutliche individuelle Variationen zwischen den Untersuchten auf. Aber es gab auch Variationen für den gesamten Gruppenmittelwert, die mit sehr niedrigen Außentemperaturen während der Solarexpositionen in Verbindung gebracht werden könnten. Bei Solarienstrahlerexpositionen analoger Dosierungen ging die Vitamin-D-Bildungseffizienz mit steigender UV-Dosis und/oder Körperfläche auf 30 % zurück, verglichen mit dem simulierten Sommersonnenspektrum. Konstante, vergleichbare Expositions- und Synthesebedingungen für die Haut in einem UV-Bestrahlungsgerät führen zu definierten Bedingungen, die sich in fast deckungsgleichem Vitamin-D-Zuwachs bei allen Probanden eines Expositionsschemas widerspiegeln. Auf analoge solare UV-Expositionen unter freiem Himmel sind diese Bedingungen nicht in jedem Fall übertragbar. Wir konnten unsere Vermutung bestätigen, dass verschiedene anatomische Hautareale sich in ihrer Vitamin-D-Bildungseffizienz stark voneinander unterscheiden. Diese variiert um bis zu 400 % und korreliert in hohem Grade signifikant mit der UV-Erythemempfindlichkeit des jeweiligen Hautareals. Die Konzentration des Provitamin D (7-Dehydrocholesterol), des Ausgangsstoffs für die Vitamin-D-Bildung in der Haut, zeigte keine Altersabhängigkeit. Mit steigender aktinischer UV-Exposition und signifikant bei 1 MED ist nach 24 h eine Erhöhung der 7-DHC-Konzentration nachzuweisen. Im Alltag haben globale Faktoren auf die UV-Personendosis (meteorologische Faktoren, solare Globalstrahlung) und persönliche Verhaltensfaktoren, die die Hautexposition beeinflussen (u.a. auch durch externer Sonnenschutzmittel), stärkeren Einfluss auf den individuellen Vitamin-D-Status im Jahresverlauf als Alter, UV-Hauttyp oder Geschlecht. Das weist die Studie in einer Personengruppe aus, deren Vitamin-D-Status dreimal jährlich über zwei Jahre verfolgt wurde. Simultan erfolgte dabei ein UV-Personenmonitoring, durch das auch die o.g. Einflussfaktoren kontinuierlich erfasst wurden. //ABSTRACT// UV-dependent vitamin D3 synthesis – balancing of UV exposure time and the production of an optimal vitamin D3 status in men The adverse health effects on human skin and eyes by UV radiation have been well known for years. They are known to the public, too. Increased exposures by the UV-B fraction of solar radiation cause e.g. sun burn as an acute skin reaction or an increased risk on skin cancer as a chronic effect. Radiation of the same spectral UV-B range is necessary to induce the essential vitamin D metabolism in men. The UV-induced vitamin D synthesis in the skin supplies the body with more than 90 % while our typical nutrition contributes no more than 10 %. These photobiological effects are diametrically opposed. Therefore, up to now there are contradictory recommendations to the public concerning the health effects of solar UV exposure. The aim of this research project was to evaluate the quantitative and qualitative relations of UV exposure and the vitamin D status in men taking into account different conditions in the population. IN RESULT, well-balanced recommendations on optimal UV exposures for the different fractions of the population should be elaborated, realizing health protection aspects against detrimental UV effects. A literature survey (updated in 2011) summarizes the current knowledge on the vitamin D metabolism, on the effects of the hormone vitamin D and on the stage of the current discussion on the optimal vitamin D status. In a number of studies of this project the effects of UV exposure on the vitamin D status (25OH-vitamin D3 und 1,25OH-vitamin D3) were investigated. Exposure parameters were the photobiologically effective UV dose (with respect to the minimal erythema dose MED = individual sun burn dose in each investigated volunteer) and the extent of the exposed skin area: face and hands (like everyday conditions) or whole body respectively. Serial UV exposures were applied by natural solar UV radiation or by simulated solar radiation or by sunbed UV lamps. All studies of the project (240 volunteers) were structured concerning UV skin type II and III, age and sex. In addition, data on the natural skin protection of the volunteers against UV radiation were measured in order to evaluate possible correlations between individual UV sensitivity and the efficiency of vitamin D synthesis. In result: In winter time, before starting the studies, the mean 25OH-vitamin D serum level of 18 ng/ml of the volunteers was in the deficiency range (< 20 ng/ml). UV exposures of 10 % MED applied twice a week vertically to face and hands caused significant increases of the 25OH-vitamin D serum level. The increase raised with higher UV doses and/or larger skin area exposed to UV radiation of the solar summer spectrum. While the increase of the 25OHvitamin D serum level in the UV cabinet was roughly independent from the basic level, under solar exposure conditions there were distinct variations between subjects as well as different outcomes for the whole group, which possibly depended on low outdoor temperatures during the solar exposures. Exposures by sunbed UV lamps lead to decreasing efficiencies in vitamin D production. An increase of the biologically effective UV dose and/or of the UV-exposed skin area decreased the vitamin D efficiency down to 30 % compared to simulated solar radiation. Because of strong differences in UV erythema sensitivity of the skin of different anatomical locations, we hypothesized similar relations in the efficiency of UV-induced vitamin D synthesis. The efficiency of UV-induced vitamin D synthesis varies up to 400 % between the anatomical locations of the body. The investigation of the content of provitamin D (7-Dehydrocholesterol), the source of the vitamin D synthesis in the skin, and of the influence of UV exposure on the level of this content results in new findings, too. Suberythemal UV exposures do not influence the 7-DHC-concentration in the skin. 1 MED leads to a significant increase of 7-DHC after 24 h. Under every day life conditions, global influences on the personal UV dose (solar global radiation, meteorological effects, outdoor temperature) and individual behaviour concerning UV exposure of the skin (among other things the use of topical sunscreens) have distinctly stronger effects on the individual vitamin D status around the year than age, UV skin type, or sex. This is suggested by the data of one of our studies, in which the vitamin D status of the volunteers was measured three times a year over two years. Simultaneously, in a personal UV monitoring the personal UV dose and the above mentioned factors were captured continuously. The results provide a large base for recommendations to the public concerning a careful use of solar UV exposures in summer in order to realize vitamin D serum levels in the optimal range. But, the results also raise a lot of questions. Answers to these questions will be essential for establishing recommendations on UV exposure and the realization of an optimal vitamin D status around the year – without an increasing risk on skin cancer due to long-term effects.
Few data are available on the exposure of children to glyphosate (Gly) in Europe. Within HBM4EU, new HBM exposure data were collected from aligned studies at five sampling sites distributed over Europe (studies: SLO CRP (SI); ORGANIKO (CY); GerES V-sub (DE); 3XG (BE); ESTEBAN (FR)). Median Gly concentrations in urine were below or around the detection limit (0.1 Ìg/L). The 95th percentiles ranged between 0.18 and 1.03 Ìg Gly/L. The ratio of AMPA (aminomethylphosphonic acid; main metabolite of Gly) to Gly at molar basis was on average 2.2 and the ratio decreased with higher Gly concentrations, suggesting that other sources of AMPA, independent of metabolism of Gly to AMPA in the monitored participants, may concurrently operate. Using reverse dosimetry and HBM exposure data from five European countries (east, west and south Europe) combined with the proposed ADI (acceptable daily intake) of EFSA for Gly of 0.1 mg/kg bw/day (based on histopathological findings in the salivary gland of rats) indicated no human health risks for Gly in the studied populations at the moment. However, the absence of a group ADI for Gly+AMPA and ongoing discussions on e.g., endocrine disrupting effects cast some uncertainty in relation to the current single substance ADI for Gly. The carcinogenic effects of Gly are still debated in the scientific community. These outcomes would influence the risk conclusions presented here. Finally, regression analyses did not find clear associations between urinary exposure biomarkers and analyzed potential exposure determinants. More information from questionnaires targeting exposure-related behavior just before the sampling is needed. © 2022 by the authors
Human Biomonitoring (HBM) of emerging chemicals gained increasing attention within the EU in recent years. After evaluating the metabolism, we established a new HBM method for ethoxyquin (EQ), a feed additive, which was banned in 2017 due to concerns regarding the possible exposure of the general population to it and its highly toxic precursor p-phenetidine. The method was applied to 250 urine samples from the Environmental Specimen Bank collected between 2000 and 2021. The major metabolite EQI was quantified in the majority of the study samples illustrating the ubiquitous exposure of the non-occupationally exposed population. A rather constant exposure was observed until 2016 with a significant decline from 2016 to 2021. This drop falls within the EU wide ban of the chemical as a feed additive from June 2017 which led to a gradual removal until its complete suspension in June 2020. The daily intake (DI) was evaluated with respect to the reported derived no-effect level (DNEL) to estimate the potential health risks from EQ exposure. The median DI of 0.0181 Ìg/kg bw/d corresponds to only 0.01 % of the DNEL. Even the observed maxima up to 13.1 Ìg/kg bw/d only accounted for 10 % of the DNEL. Nevertheless, the values suggest a general exposure with the risk of higher burden in a low fraction of the population. In regard to the EQ associated intake of the carcinogen and suspected mutagen p-phenetidine, this level of exposure cannot be evaluated as safe. The recent decrease and the broad exposure substantiate the need for future HBM campaigns in population representative studies to further investigate the observed reductions, potentially find highly exposed subgroups and clarify the impact of the ban as feed additive on EQ exposure. © 2023 The Author(s)
In recent years, exposure to parabens has become more of a concern because of evidence of ubiquitous exposure in the general population, combined with evidence of their potency as endocrine disruptors. New human metabolism data from oral exposure experiments enable us to back calculate daily paraben intakes from urinary paraben levels. We report daily intakes (DIs) for six parabens based on 660 24h urine samples from the German Environmental Specimen Bank collected between 1995 and 2012. Median DI values ranged between 1.1Ţg/kg bw/day for iso-butyl paraben and 47.5Ţg/kg bw/day for methyl paraben. The calculated DIs were compared with acceptable levels of exposure to evaluate the hazard quotients (HQs) that indicate that acceptable exposure is exceeded for values of >1. Approximately 5% of our study population exceeded this threshold for individual paraben exposure. The hazard index (HI) that takes into account the cumulative risk of adverse estrogenic effects was 1.3 at the 95th percentile and 4.4 at maximum intakes, mainly driven by n-propyl paraben exposure. HI values of >1 indicate some level of concern. However, we have to point out that we applied most conservative assumptions in the HQ/HI calculations. Also, major exposure reduction measures were enacted in the European Union after 2012. Quelle: www.nature.com
4-methylbenzylidene camphor (4-MBC) is used as a UV-B filter in cosmetics. Two oxidized metabolites of 4-MBC - 3-(4-carboxybenzylidene)camphor (cx-MBC) and 3-(4-carboxybenzylidene)-6-hydroxycamphor (cx-MBC-OH) - were analyzed in 250 24-h urine samples from young adults in Germany. The samples were from the German Environmental Specimen Bank (ESB) and represented exposure in the years 1995, 2005, 2010, 2015 and 2019. A UHPLC-MS/MS method enabled the sensitive determination of both metabolites, with limits of quantifi cation at 0.15 mikrogL-1 (cx-MBC) and 0.30 mikrogL-1 (cx-MBC-OH), respectively. A temporal trend of the internal exposure to 4-MBC was clearly noticeable. The metabolite cx-MBC was frequently quantifiable at the beginning of the period: in 70% of the samples in 1995, and 56% in 2005. After 2005, urinary concentrations and detection rates of cx-MBC dropped to reach very low levels. In 2015 and 2019, the detection rate was only 2% and 0%, respectively. A similar trend was observed for cx-MBC-OH, though overall, this metabolite was detected less often and at lower concentration levels than cx-MBC. Nowadays, measurable levels of urinary 4-MBC metabolites are an extremely rare occurrence in Germany. These trends are consistent with the history of 4-MBC use by the cosmetic industry. The highest measured individual concentration of 16.20 mikrogL-1 (in a sample of the year 2005) was still more than 30 times below the health-based guidance value (HBM-I). An investigation of the ratios between both metabolites uncovered several features of the 4-MBC metabolism which have been essentially overlooked until now. In particular, stereochemical aspects should be explored in future studies. As urine was collected in autumn/winter in Northwestern Germany, the 4-MBC metabolites measured prob ably do not arise from sunscreen products in a narrow sense. They rather may reveal the use of other skin care products containing 4-MBC for UV protection as an added feature. © 2023 Elsevier
Indicators are required to monitor the progress of resource and circular economy policies. The German Sustainable Development Strategy and Resource Efficiency Program already include a number of indicators for mapping Germany's resource use and socio-economic metabolism. However, currently used indicators only include a subset of natural resources and often lack an impact evaluation (e.g., considering resource scarcity or environmental relevance). Resource and environmental footprints indirectly caused through the trade of goods have so far only partly been considered by German resource policy and in official statistics. As a result, burden shifting between different resource categories, world regions, or environmental effects can remain undetected. To fill this gap, we discuss the overall scope of natural resource monitoring in Germany and review existing resource indicators evaluating them against a set of predefined criteria. We then propose a possible monitoring framework for Germany consisting of a materials-layer (the focus of resource and circular economy policies to date) for the evaluation of material flows and stocks, and corresponding water, land, and emissions-layers which should be monitored simultaneously to track contributions to the overarching objectives of resource and circular economy policies. Possible indicators and data sources are discussed and an outlook for future research provided. © 2021 The Authors
Background For evaluating the fate of xenobiotics in the environment, a variety of degradation or environmental metabolism experiments are routinely conducted. The data generated in such experiments are evaluated by optimizing the parameters of kinetic models in a way that the model simulation fits the data. No comparison of the main software tools currently in use has been published to date. This article shows a comparison of numerical results as well as an overall, somewhat subjective comparison based on a scoring system using a set of criteria. The scoring was separately performed for two types of uses. Uses of type I are routine evaluations involving standard kinetic models and up to three metabolites in a single compartment. Evaluations involving non-standard model components, more than three metabolites or more than a single compartment belong to use type II. For use type I, usability is most important, while the flexibility of the model definition is most important for use type II. Results Test datasets were assembled that can be used to compare the numerical results for different software tools. These datasets can also be used to ensure that no unintended or erroneous behaviour is introduced in newer versions. In the comparison of numerical results, good agreement between the parameter estimates was observed for datasets with up to three metabolites. For the now unmaintained reference software DegKinManager/ModelMaker, and for OpenModel which is still under development, user options were identified that should be taken care of in order to obtain results that are as reliable as possible. Based on the scoring system mentioned above, the software tools gmkin, KinGUII and CAKE received the best scores for use type I. Out of the 15 software packages compared with respect to use type II, again gmkin and KinGUII were the first two, followed by the script based tool mkin, which is the technical basis for gmkin, and by OpenModel. Conclusions Based on the evaluation using the system of criteria mentioned above and the comparison of numerical results for the suite of test datasets, the software tools gmkin, KinGUII and CAKE are recommended for use type I, and gmkin and KinGUII for use type II. For users that prefer to work with scripts instead of graphical user interfaces, mkin is recommended. For future software evaluations, it is recommended to include a measure for the total time that a typical user needs for a kinetic evaluation into the scoring scheme. It is the hope of the authors that the publication of test data, source code and overall rankings foster the evolution of useful and reliable software in the field. © The Author(s) 2018
The antioxidant 2,6-di-tert-butyl-4-methylphenol (butylated hydroxytoluene, BHT) is used ubiquitously in food, cosmetics, pharmaceuticals, fuels, plastics, rubbers and many other products. Therefore, exposure of the general population to this substance is likely. We analyzed the BHT metabolite 3,5-di-tert-butyl-4-hydroxybenzoic acid ("BHT acid") in 24-h urine samples from the German Environmental Specimen Bank with the aim of gaining a better understanding of the internal burden of BHT in young nonspecifically exposed adults. The study population consisted of students between 20 and 29 years of age at the time of sampling, all from Halle/Saale in Central Germany. In total, 329 samples collected in the years 2000, 2004, 2008, 2012, 2015, and 2018 were measured by ultra high performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS). BHT acid was detected above the limit of quantification (0.2 My g/L) in 98% of the samples. The median of the measured concentrations was 1.06 My g/L and 1.24 My g/g creatinine respectively, the median of the daily excretion was 1.76 My g/24 h and - additionally normalized for body weight - 26.8 ng/24 h * kg bw respectively. The corresponding 90th percentiles were 3.28 My g/L, 3.91 My g/g creatinine, 5.05 My g/24 h, and 81.9 ng/24 h * kg bw. Medians of creatinine-corrected values were slightly higher in women than in men, while the opposite situation was observed for the volume concentrations and the 24-h excretion values (not corrected for body weight). Values simultaneously normalized both for 24-h excretion and body weight did not exhibit any significant differences between males and females, probably indicating a virtually identical magnitude of exposure for both genders. The background exposure of the investigated population was found to be largely constant since the year 2000, with only weak temporal trends at most. Daily intakes were estimated from excretion values and found to be largely below the acceptable daily intake (ADI) of BHT at 0.25 mg/kg bw: our worst-case estimate is a daily BHT intake of approximately 0.1 mg/kg bw at the 95th percentile level. However, these intake assessments rely on very limited quantitative data regarding human metabolism of BHT. © 2020 Elsevier GmbH. All rights reserved.
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