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Wölz J Grosshans K Streck G Schulze T Rastall A Erdinger L Brack W Fleig M Kühlers D Braunbeck T Hollert H 《Chemosphere》2011,85(5):717-723
Bankside groundwater is widely used as drinking water resource and, therefore, contamination has to be avoided. In the European Union groundwater protection is explicit subject to Water Framework Directive. While groundwater pollution may originate from different sources, this study investigated on impacts via flood events.Groundwater was sampled with increasing distance to the river Rhine near Karlsruhe, Germany. Samples were HPLC-MS-MS analyzed for the river contaminant carbamazepine to indicate river water infiltration, giving permanent presence in 250 m distance to the river (14-47 μg L−1). Following a flood event, concentrations of about 16-20 μg L−1 could also be detected in a distance of 750 m to the river. Furthermore, estrogenic activity as determined with the Yeast Estrogen Screen assay was determined to increase up to a 17β-ethinylestradiol equivalent concentration (E-EQ) = 2.9 ng L−1 near the river, while activity was initially measured following the flood with up to E-EQ = 2.6 ng L−1 in 750 m distance. Detections were delayed with increasing distance to the river indicating river water expansion into the aquifer.Flood suspended matter and floodplain soil were fractionated and analyzed for estrogenic activity in parallel giving up to 1.4 ng g−1 and up to 0.7 ng g−1, respectively. Target analysis focusing on known estrogenic active substances only explained <1% of measured activities.Nevertheless, river water infiltration was shown deep into bankside groundwater, thus, impacting groundwater quality. Therefore, flood events have to be in the focus when aiming for groundwater and drinking water protection as well as for implementation of Water Framework Directive. 相似文献
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Lebo JA Almeida FV Cranor WL Petty JD Huckins JN Rastall A Alvarez DA Mogensen BB Johnson BT 《Chemosphere》2004,54(8):1217-1224
Analyses of triolein-containing semipermeable membrane devices (SPMDs) have sometimes been impeded by interferences caused by impurities endemic to triolein that codialyze with the analytes. Oleic acid and methyl oleate have been the most troublesome of these impurities because of their relatively high concentrations in triolein and because significant residues of both can persist even after size exclusion chromatographic (SEC) fractionation. These residues have also been blamed for false-positive signals during bioindicator testing of SPMD dialysates. To prevent these problems, a simple, cost-effective procedure was developed for purifying triolein destined for use in SPMDs: the bulk triolein is repeatedly (6x) partitioned against methanol. Tests of the procedure show that 14C-oleic acid is completely removed from the triolein. After SEC fractionation, dialysates of standard-size SPMDs made with the purified triolein contain less than 5 microg of methyl oleate as compared to sometimes more than 500 microg for dialysates (also after SEC) of SPMDs made with unpurified triolein. Gas chromatographic analyses with flame ionization and electron capture detection show that the purification treatment also greatly reduces the number and size of peaks caused by unidentified contaminants in the triolein. Microtox basic assay of dialysates of SPMDs shows that those made with the purified triolein have lower acute toxicities than dialysates of SPMDs made with unpurified triolein. Yeast estrogen screen (YES) testing of SPMDs fabricated with unpurified and purified triolein demonstrates that the purification process removes all background estrogenic activity. 相似文献
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A holistic passive integrative sampling approach for assessing the presence and potential impacts of waterborne environmental contaminants 总被引:4,自引:0,他引:4
Petty JD Huckins JN Alvarez DA Brumbaugh WG Cranor WL Gale RW Rastall AC Jones-Lepp TL Leiker TJ Rostad CE Furlong ET 《Chemosphere》2004,54(6):695-705
As an integral part of our continuing research in environmental quality assessment approaches, we have developed a variety of passive integrative sampling devices widely applicable for use in defining the presence and potential impacts of a broad array of contaminants. The semipermeable membrane device has gained widespread use for sampling hydrophobic chemicals from water and air, the polar organic chemical integrative sampler is applicable for sequestering waterborne hydrophilic organic chemicals, the stabilized liquid membrane device is used to integratively sample waterborne ionic metals, and the passive integrative mercury sampler is applicable for sampling vapor phase or dissolved neutral mercury species. This suite of integrative samplers forms the basis for a new passive sampling approach for assessing the presence and potential toxicological significance of a broad spectrum of environmental contaminants. In a proof-of-concept study, three of our four passive integrative samplers were used to assess the presence of a wide variety of contaminants in the waters of a constructed wetland, and to determine the effectiveness of the constructed wetland in removing contaminants. The wetland is used for final polishing of secondary-treatment municipal wastewater and the effluent is used as a source of water for a state wildlife area. Numerous contaminants, including organochlorine pesticides, polycyclic aromatic hydrocarbons, organophosphate pesticides, and pharmaceutical chemicals (e.g., ibuprofen, oxindole, etc.) were detected in the wastewater. Herein we summarize the results of the analysis of the field-deployed samplers and demonstrate the utility of this holistic approach. 相似文献
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Rastall AC Getting D Goddard J Roberts DR Erdinger L 《Environmental science and pollution research international》2006,13(4):256-267
Goal, Scope and Background
Some anthropogenic pollutants posses the capacity to disrupt endogenous control of developmental and reproductive processes
in aquatic biota by activating estrogen receptors. Many anthropogenic estrogen receptor agonists (ERAs) are hydrophobic and
will therefore readily partition into the abiotic organic carbon phases present in natural waters. This partitioning process
effectively reduces the proportion of ERAs readily available for bioconcentration by aquatic biota. Results from some studies
have suggested that for many aquatic species, bioconcentration of the freely-dissolved fraction may be the principal route
of uptake for hydrophobic pollutants with logarithm n-octanol/water partition coefficient (log Kow) values less than approximately
6.0, which includes the majority of known anthropogenic ERAs. The detection and identification of freely-dissolved readily
bioconcentratable ERAs is therefore an important aspect of exposure and risk assessment. However, most studies use conventional
techniques to sample total ERA concentrations and in doing so frequently fail to account for bioconcentration of the freely-dissolved
fraction. The aim of the current study was to couple the biomimetic sampling properties of semipermeable membrane devices
(SPMDs) to a bioassay-directed chemical analysis (BDCA) scheme for the detection and identification of readily bioconcentratable
ERAs in surface waters.
Methods
SPMDs were constructed and deployed at a number of sites in Germany and the UK. Following the dialytic recovery of target
compounds and size exclusion chromatographic clean-up, SPMD samples were fractionated using a reverse-phase HPLC method calibrated
to provide an estimation of target analyte log Kow. A portion of each HPLC fraction was then subjected to the yeast estrogen
screen (YES) to determine estrogenic potential. Results were plotted in the form of 'estrograms' which displayed profiles
of estrogenic potential as a function of HPLC retention time (i.e. hydrophobicity) for each of the samples. Where significant
activity was elicited in the YES, the remaining portion of the respective active fraction was subjected to GC-MS analysis
in an attempt to identify the ERAs present.
Results and Discussion
Estrograms from each of the field samples showed that readily bioconcentratable ERAs were present at each of the sampling
sites. Estimated log Kow values for the various active fractions ranged from 1.92 to 8.63. For some samples, estrogenic potential
was associated with a relatively narrow range of log Kow values whilst in others estrogenic potential was more widely distributed
across the respective estrograms. ERAs identified in active fractions included some benzophenones, various nonylphenol isomers,
benzyl butyl phthalate, dehydroabietic acid, sitosterol, 3-(4-methylbenzylidine)camphor (4-MBC) and 6-acetyl-1,1,2,4,4,7-hexamethyltetralin
(AHTN). Other tentatively identified compounds which may have contributed to the observed YES activity included various polycyclic
aromatic hydrocarbons (PAHs) and their alkylated derivatives, methylated benzylphenols, various alkylphenols and dialkylphenols.
However, potential ERAs present in some active fractions remain unidentified.
Conclusions and Outlook
Our results show that SPMD-YES-based BDCA can be used to detect and identify readily bioconcentratable ERAs in surface waters.
As such, this biomimetic approach can be employed as an alternative to conventional methodologies to provide investigators
with a more environmentally relevant insight into the distribution and identity of ERAs in surface waters. The use of alternative
bioassays also has the potential to expand SPMD-based BDCA to include a wide range of toxicological endpoints. Improvements
to the analytical methodology used to identify ERAs or other target compounds in active fractions in the current study could
greatly enhance the applicability of the methodology to risk assessment and monitoring programmes. 相似文献
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Toxicity, dioxin-like activities, and endocrine effects of DDT metabolites—DDA, DDMU, DDMS, and DDCN
Wetterauer B Ricking M Otte JC Hallare AV Rastall A Erdinger L Schwarzbauer J Braunbeck T Hollert H 《Environmental science and pollution research international》2012,19(2):403-415
Background, aim, and scope
2,2-bis(chlorophenyl)-1,1,1-trichloroethane (DDT) metabolites, other than those routinely measured [i.e., 2,2-bis(chlorophenyl)-1,1-dichloroethylene (DDE) and 2,2-bis(chlorophenyl)-1,1-dichloroethane (DDD)], have recently been detected in elevated concentrations not only in the surface water of Teltow Canal, Berlin, but also in sediment samples from Elbe tributaries (e.g., Mulde and Havel/Spree). This was paralleled by recent reports that multiple other metabolites could emerge from the degradation of parent DDT by naturally occurring organisms or by interaction with some heavy metals. Nevertheless, only very few data on the biological activities of these metabolites are available to date. The objective of this communication is to evaluate, for the first time, the cytotoxicity, dioxin-like activity, and estrogenicity of the least-studied DDT metabolites. 相似文献9.
Keiter S Rastall A Kosmehl T Wurm K Erdinger L Braunbeck T Hollert H 《Environmental science and pollution research international》2006,13(5):308-319
Goals, Scope and Background Fish populations, especially those of the grayling (Thymallus thymallus), have declined over the last two decades in the
upper Danube River between Sigmaringen and Ulm, despite intensive and continuous stocking and improvement of water quality
since the 1970s. Similar problems have been reported for other rivers, e.g. in Switzerland, Great Britain, the United States
and Canada. In order to assess if ecotoxicological effects might be related to the decline in fish catch at the upper Danube
River, sediment, suspended matter and waste water samples from sewage treatment plants were collected at selected locations
and analyzed in a bioanalytical approach using a battery of bioassays. The results of this pilot study will be used to decide
if a comprehensive weight-of-evidence study is needed.
Methods Freeze-dried sediments and suspended particulate matters were extracted with acetone in a Soxhlet apparatus. Organic pollutants
from sewage water were concentrated using XAD-resins. In order to investigate the ecotoxicological burden, the following bioassays
were used: (1) neutral red assay with RTL-W1 cells (cytotoxicity), (2) comet assay with RTLW1 cells (genotoxicity), (3) Arthrobacter
globiformis dehydrogenase assay (toxicity to bacteria), (4) yeast estrogen screen assay (endocrine disruption), (5) fish egg
assay with the zebrafish (Danio rerio; embryo toxicity) and (6) Ames test with TA98 (mutagenicity).
Results and Discussion The results of the in vitro tests elucidated a considerable genotoxic, cytotoxic, mutagenic, bacteriotoxic, embryotoxic and
estrogenic burden in the upper Danube River, although with a very inhomogeneous distribution of effects. The samples taken
from Riedlingen, for example, induced low embryo toxicity, but the second highest 17β-estradiol equivalent concentration (1.8
ng/L). Using the fish egg assay with native sediments, a broad range of embryotoxic effects could be elucidated, with clear-cut
dose-response relationships for the embryotoxic effects of contaminated sediments. With native sediments, embryotoxicity was
clearly higher than with corresponding pore waters, thus corroborating the view that – at least for fish eggs – the bioavailability
of particle-bound lipophilic substances in native sediments is higher than generally assumed. The effect observed most frequently
in the fish egg assay was a developmental delay. A comparison of our own results with locations along the rivers Rhine and
Neckar demonstrated similar or even higher ranges of ecotoxicological burdens in the Danube River.
Conclusions The complex pattern of ecotoxicological effects caused by environmental samples from the Danube River, when assessed in an
in vitro biotest battery using both acute and more specific endpoints, showed that integration of different endpoints is essential
for appropriate hazard assessment. Overall, the ecotoxicological hazard potential shown has indeed to be considered as one
potential reason for the decline in fish catches at the upper Danube River. However, based on the results of this pilot study,
it is not possible to elucidate that chemically induced alterations are responsible for the fish decline.
Recommendations and Perspective . In order to confirm the ecological relevance of the in vitro results for the situation in the field and especially for the
decline of the grayling and other fishes, further integrated investigations are required. For linking the weight of evidence
obtained by in vitro assays and fish population investigations, the application of additional, more specific biomarkers (e.g.
vitellogenin induction, EROD and micronucleus assay) has been initiated in fish taken from the field as well as in situ investigations. 相似文献
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