Zielsetzung: Angaben ueber physiologische Wirkung wasserloeslicher Fraktionen von Rohoelen im Hinblick auf Synergismus mit 'natuerlichen' entwicklungserschwerenden Umweltbedingungen. 1. Laborexperimente zur Abgrenzung von sublet. und subterratogenen Konzentrationen und Dosen. Registrierung von embryonaler Sterblichkeit, Missbildung, Schluepferfolg und Vitalitaet der Larven. Vergleichsbeobachtungen ueber Schwimmverhalten, Nahrungsaufnahme und Wachstumsraten. 2. Chemische Analysen der Organismen: Backgroundkontamierung der Fischovarien. Messung der Ad- und Absorption am Chorion und im Gewebe. Messung der physiologischen Belastungen (Gesamtstoffwechsel), spezielle Untersuchungen ueber Einfluss adsorbierter Stoffe. Untersuchungen ueber ontogenetische Entwicklung der Faehigkeiten zur Metabolierung und Exkretion von Kohlenwasserstoffen. Messungen ueber Rohoel-Loesungskinetik und Alterung von Rohoel-Seewasser-Extrakten.
Phthalates 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.
Over the last twenty-five years it has become evident that exposure to several phthalates can have adverse effects on human health, such as endocrine disruption. This led to a series of EU regulations that resulted in a decrease in the production volumes of the restricted phthalates and an increased production of substitutes. The current study describes the impact of regulations and changes in production and use of phthalates and their substitutes on internal exposure patterns in two European populations since the beginning of the 2000'ies. Using harmonised data from young adults in Denmark (Danish Young Men Study, n = 1,063, spot urine) and Germany (Environmental Specimen Bank, n = 878, 24-h urine) with repeated cross-sectional design (3-11 cycles per biomarker) we applied Locally Estimated Scatterplot Smoothing (LOESS) and Generalized Linear Models (GLMs) to estimate time trends and the role of covariates on the trend (e.g. age, BMI). Time trends of daily excretion (mikrog/24h) are comparable between the two samples for the regulated (DEHP, BBzP, DiNP, DnBP, DiBP, DiDP/DPHP) as well as the non-regulated substances (DMP, DEP, DINCH, DEHTP) although the rate of change differ for some of the compounds. GLM results indicate that the daily excretion of the most regulated phthalates has decreased over time (DEHP yearly about 12-16%, BBzP 5%, DnBP 0.3-17%, and DiBP 4-12%). Interestingly, also the non-regulated phthalates DMP and DEP decreased by 6-18% per year. In sharp contrast, the phthalate substitutes DINCH and DEHTP show very steep annual increases (~10-68% and ~100%, respectively) between 2009 and 2017. We did not find an effect of age, sex, BMI, or education on the time trend. The present study provides comparable insights into how exposure to phthalates and two of their substitutes have changed over the last two decades in Germany and Denmark. © 2022 The Authors
The mycotoxin deoxynivalenol (DON) is a frequently found contaminant in cereals and cereal-based products. As a German contribution to the European Joint Programme HBM4EU, we analysed the total DON concentration (tDON) in 24-h urine samples from the German Environmental Specimen Bank (ESB). In total, 360 samples collected in 1996, 2001, 2006, 2011, 2016, and 2021 from young adults in Muenster (Germany), were measured by high performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) after enzymatic deconjugation of the glucuronide metabolites. tDON was found in concentrations above the lower limit of quantification (0.3 (micro)g/L) in 99% of the samples. Medians of the measured concentrations and the daily excretion were 4.3 (micro)g/L and 7.9 (micro)g/24 h, respectively. For only nine participants, urinary tDON concentrations exceeded the provisional Human biomonitoring guidance value (HBM GV) of 23 (micro)g/L. Urinary tDON concentrations were significantly higher for male participants. However, 24-h excretion values normalized to the participant's body weight did not exhibit any significant difference between males and females and the magnitude remained unchanged over the sampling years with exception of the sampling year 2001. Daily intakes were estimated from excretion values. Exceedance of the tolerable daily intake (TDI) of 1 (micro)g/kg bw per day was observed for less than 1% of all participants. TDI exceedances were only present in the sampling year 2001 and not in more recent sampling years while exceedance of the HBM guidance value was also observed in 2011 and 2021. © 2023 The Authors
The UV filters octocrylene (OC) and 2-ethylhexyl salicylate (EHS) are commonly used in sunscreens and frequently detected in environmental media. However, knowledge on human exposures is scarce. In this human biomonitoring (HBM) study, we analyzed concentrations of exposure biomarkers specific to OC (CPAA, DOCCA, 5OH-OC) and EHS (5OH-EHS, 5oxo-EHS, 5cx-EPS) in 24-h urine samples (n=420) from the German Environmental Specimen Bank (ESB). These samples were collected from German students (20-29 years; 30 males/30 females per year) between 1996 and 2020 (4-year intervals; collection in winter). We found continuously increasing OC and EHS exposures (Jonckheere-Terpstra; p < 0.001) documented by very few to no samples with concentrations of the most sensitive biomarkers CPAA and 5cx-EPS above the limit of quantification (LOQ) in 1996 (5 % and 0 %, respectively) and reaching 100 % and 93 % above the LOQ in 2016, with median concentrations of 4.79 and 0.071 (micro)g/L, respectively. In 2020, biomarker concentrations slightly decreased to 3.12 (micro)g/L CPAA (97 %>LOQ) and 0.060 (micro)g/L 5cx-EPS (88 %>LOQ). This general trend was confirmed by the other biomarkers, however at lower detection rates. Based on metabolite excretion in the 24-h urine samples and human toxicokinetic data, we calculated maximum daily intakes (DI) of 17 (micro)g/(kg bw * d) OC and 59 (micro)g/(kg bw * d) EHS. Based on a derived no-effect level (DNEL) of 0.8 mg/(kg bw * d), the OC exposures of individuals in our study did not indicate any health risk. Similarly, for EHS all biomarker concentrations were well below the HBM-I values of 12 (micro)g/L 5OH-EHS and 11 (micro)g/L 5cx-EPS. Our data proves the general applicability of specific OC and EHS metabolites for HBM in the general population and shows clearly increasing exposures. Higher (co-)exposures must be expected in populations with increased sunscreen use such as (summer) vacationers, children and outdoor workers. © 2023 The Author(s).
As highlighted in the Minamata Convention, Mercury (Hg) in its various forms poses a substantial risk to human health and the environment. The health relevance of Hg is also recognized by the European Human Biomonitoring Initiative (HBM4EU), which classifies Hg as a priority substance, since considerable knowledge and data gaps on Hg exposure levels and their changes over time still exist in Europe. The German Environmental Specimen Bank (German ESB) provides valuable policy relevant data and long-term trends of substance exposure on a national level for international comparison and evaluation. In this study we analysed data of the German ESB on Hg exposure of young adults aged 20 to 29 including data on urinary Hg levels from 1995 to 2018 and whole blood Hg levels from 2001 to 2010. Results show a clear decrease in both, about 86% in urine total daily Hg excretion from 1995 (0.76 (micro)g/L) to 2018 (0.11 (micro)g/L) (n = 10,069) and about 57% in blood concentrations of Hg from 2001 (1.76 (micro)g/L) to 2010 (0.77 (micro)g/L) (n = 4085). Over the investigated timeframe only a few values exceeded the toxicologically derived health based guidance value HBM I for blood and urine, with these exceedances decreasing over time in line with the general trend. The factors mostly influencing Hg excretion identified in this study are dental amalgam as well as fish and seafood consumption. Besides other factors (e.g. age and sex), also airborne Hg exposure appears to be a low but evident influencing factor in Germany. Although a considerable decrease in internal Hg exposure is recognized in the last decades, the current low-level exposure may cause adverse health effects especially to vulnerable groups such as pregnant women and children. To further elucidate and evaluate current exposure sources and to reduce human exposure to Hg, continuous environmental and human biomonitoring is needed. © 2022 The Authors.
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. © 2021 Elsevier GmbH.
Parasiticides are veterinary pharmaceuticals very frequently used in pasture animals. Particularly substances of the classes of avermectins and milbemycins are very common. These substances are highly toxic to non-target organisms, often stable in the environment (persistent) and may potentially accumulative in organisms. The present project contributes to filling environmental data gaps for avermectins and milbemycins. In addition, risk management strategies for parasiticides used in pasture animals were evaluated with regard to their efficacy and practicability reducing the risk to dung or soil organisms.
This data set contains measures of energy-use efficiency, energy flow, and energy storage in units of dry biomass that quantify the multitrophic ecosystem functioning realized in grassland ecosystems of differing plant diversity. Given are both the measures integrated over whole ecosystems (total network measures) as well as the energy dynamics associated with individual ecosystem compartments including the entire biological community and detrital compartments across the above- and belowground parts of the ecosystem. Data presented here is from the Main Experiment plots of a large grassland biodiversity experiment (the Jena Experiment, see further details below). In the main experiment, 82 grassland plots of 20 x 20 m were established from a pool of 60 species belonging to four functional groups (grasses, legumes, tall and small herbs). In May 2002, varying numbers of plant species from this species pool were sown into the plots to create a gradient of plant species richness (1, 2, 4, 8, 16 and 60 species) and functional richness (1, 2, 3, 4 functional groups). Study plots are grouped in four blocks in parallel to the river in order to account for any effect of a gradient in abiotic soil properties. Each block contains an equal number of plots of each plant species richness and plant functional group richness level. Plots were maintained in general by bi-annual weeding and mowing. Since 2010, plot size was reduced to 5.5 x 6 m and plots were weeded three times per year. Trophic-network models were constructed for 80 of the experimental plots, and represent the ecosystem energy budget in the currency of dry-mass (g m-2 for standing stocks and g m-2 d-1 for flows). All trophic networks have the same topology, but they differ in the estimated size of the standing stock biomass of individual compartments (g m-2) and flows among the compartments (g m-2 d-1). Each trophic network contains twelve ecosystem compartments representing distinct trophic groups of the above- and belowground parts of the ecosystem (i.e., plants, soil microbial community, and above- and belowground herbivores, carnivores, omnivores, decomposers, all represented by invertebrate macro- and mesofauna) and detrital pools (i.e., surface litter and soil organic matter). Vertebrates were not considered in our study due to limitations of data availability and because the impact of resident vertebrates in our experimental system is expected to be minimal. Larger grazing vertebrates were excluded by a fence around the field site, though there was some occasional grazing by voles. Compartments are connected by 41 flows. Flows (fluxes) constitute 30 internal flows within the system, namely feeding (herbivory, predation, decomposition), excretion, mortality, and mechanical transformation of surface litter due to bioturbation plus eleven 11 external flows, i.e. one input (flows entering the system, namely carbon uptake by plants) and ten output flows (flows leaving the system, namely respiration losses). The ecosystem inflow (a flow entering the system) and outflows (flows leaving the system) represent carbon uptake and respiration losses, respectively. In the case of consumer groups, the food consumed (compartment-wide input flow) is further split into excretion (not assimilated organic material that is returned to detrital pools in the form of fecesfaeces) and assimilated organic material, which is further split into respiration (energy lost out of the system to the environment) and biomass production, which is further consumed by higher trophic levels due to predation or returned to detrital pools in the form of mortality (natural mortality or prey residues). In case of detrital pools (i.e. surface litter and soil organic matter), the input flows are in the form of excretion and mortality from the biota compartments, and output flows are in the form of feeding by decomposers and soil microorganisms (i.e. decomposition). Surface litter and soil organic matter are connected by flows in the form of burrowing (mechanical transportation) of organic material from the surface to the soil by soil fauna. Organism immigration and emigration are not considered in our study due to limited data availability. Flows were quantified using resource processing rates (i.e. the feeding rates at which material is taken from a source) multiplied with the standing biomass of the respective source compartment. To approximate resource processing rates, different approaches were used: (i) experimental measurements (namely the aboveground decomposition, fauna burial activity (bioturbation), microbial respiration, and aboveground herbivory and predation rates); (ii) allometric equations scaled by individual body mass, environmental temperature and phylogenetic group (for the above- and belowground fauna respiration rates and plant respiration); (iii) assimilation rates scaled by diet type (for quantification of belowground fauna excretion and natural mortality); (iv) literature-based rates scaled by biomass of trophic groups (for microbial mortality); and (v) mass-balance assumptions (carbon uptake, plant and aboveground fauna mortality, belowground decomposition, belowground herbivory, and belowground predation). Mass-balance assumption means that the flows are calculated assuming that resource inputs into the compartment (i.e. feeding) balance the rate at which material is lost (i.e. the sum of through excretion, respiration, predation, and natural death). We used constrained nonlinear multivariable optimization to perturb the initial flow rates estimated from the various sources. We assigned confidence ratings for each flow rate, reflecting the quality of empirical data it is based on. We then used the 'fmincon' function from Matlab's optimization toolbox, which utilizes the standard Moore-Penrose pseudoinverse approach to achieve a balanced steady state ecological network model that best reflects the collected field data. Measured data used to parameterize the trophic network models were collected mostly in the year 2010. Network-wide measures that quantify proxies for different aspects of multitrophic ecosystem functioning were calculated for each experimental plot using the 'enaR' package in R. In particular, total energy flow was measured as the sum of all flows through each ecosystem compartment. Flow uniformity was calculated as the ratio of the mean of summed flows through each individual ecosystem compartment divided by the standard deviation of these means. Total-network standing biomass was determined as the sum of standing biomass across all ecosystem compartments. Community maintenance costs were calculated as the ratio of community-wide respiration related to community-wide biomass.
The copepod Temora longicornis depends on constant prey availability. Given that climate change may induce food regime shifts, our research goal was to understand copepod energy allocation in relation to diet quality. The working hypothesis was that Temora performs better on the diet whose elemental ratio is closest to its own. Diatoms (Diat) and dinoflagellates (Dino) cultured in nutrient-replete (+) and nitrogen-depleted (-) conditions were fed to the copepods. Ingestion, respiration, excretion, and egg and faecal pellet production rates were measured. Carbon (C) and nitrogen (N) budgets were built to investigate differences in dietary C and N partitioning. Copepods fed with nitrogen-depleted diatoms (Diat-), which had the most different C:N ratio to that of T. longicornis, had high metabolic losses and low growth. In contrast, copepods fed with nitrogen-rich dinoflagellates (Dino+) of closer C:N ratio had high metabolic losses, but the highest investment into somatic and reproductive tissue. The results indicate that, under the current climate scenario and nutrient-replete conditions, dinoflagellates are a better food source for T. longicornis. Furthermore, ingestion, respiration, and faecal pellet integrity are adversely affected by low quality food; and egestion is a main pathway in copepods for eliminating excess carbon.
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