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Rastall AC Neziri A Vukovic Z Jung C Mijovic S Hollert H Nikcevic S Erdinger L 《Environmental science and pollution research international》2004,11(4):240-253
GOAL, SCOPE AND BACKGROUND: Lake Shkodra/Skadar is the largest lake in the Balkans region and located on the border between Albania to the south and Montenegro to the north. Because of the wide range of endemic, rare or endangered plant and animal species it supports, Lake Shkodra/Skadar and its extensive associated wetlands are internationally recognised as a site of significance and importance (Ramsar site). In recent years, social and economic changes in both Albania and Montenegro have lead to unprecedented levels of urban and industrial effluent entering the lake. Of particular concern is the increasing input of toxic hydrophobic organic pollutants (HOPs) into the lake and the degree to which these compounds are available for uptake by aquatic biota. Semipermeable membrane devices (SPMDs) have been shown to sample the readily bioavailable fraction (dissolved phase) of waterborne HOPs and in doing so provide relevant data for exposure assessment. The aim of the current study was to use SPMD-based sampling in conjunction with appropriate bioassays and chemical analysis to identify readily bioavailable HOPs in the lake. METHODS: SPMDs were constructed and deployed at three sites in the Albanian sector and three sites in the Montenegrin sector of Lake Skadar/Shkodra for 21 days. Following the dialytic recovery of target analytes and size exclusion chromatographic clean-up, aliquots of SPMD samples were subjected to GC-MS scan analysis for major components, GC-MS SIM analysis for 16 priority pollutant polycyclic aromatic hydrocarbons (PP-PAHs) and assayed for EROD-inducing, estrogenic and mutagenic potential using rainbow trout liver cells (RTL-W1), the yeast estrogen screen (YES) and the Ames Test, respectively. RESULTS AND DISCUSSION: A total of 39 compounds were tentatively identified in SPMD samples from the six sampling sites. Alkylated PAHs were the most abundant and ubiquitous compounds present along with various sterols and sterol derivatives. Numerous other compounds remain unidentified. 15 of the 16 targeted PP-PAHs were present in samples from one or more of the sampling sites indicating these compounds are both readily bioavailable and widely distributed in Lake Shkodra/Skadar. Total PP-PAH concentrations ranged between 3991 ng/SPMD and 10695 ng/SPMD. Bioassays carried out on SPMD samples revealed significant EROD-inducing and estrogenic potential at five of the six sampling sites indicating toxicologically relevant compounds are readily available for uptake by resident aquatic biota. EROD-inducing potential was positively correlated with targeted PP-PAH concentration (r2 = 0.74). However, comparison of bioassay- and analytically-derived toxicity equivalents revealed targeted PP-PAHs were responsible for less than 0.06% of the total EROD-inducing potential. CONCLUSIONS AND OUTLOOK: The combination of SPMD-based sampling with appropriate bioassays and chemical analysis provided an effective tool for the identification of environmentally relevant waterborne pollutants in Lake Shkodra/Skadar. Our results show that toxicologically relevant HOPs including EROD-inducing and potentially estrogenic compounds are widely distributed in the lake and readily available for uptake by aquatic biota. Our results also suggest that alkylated PAHs rather than parent compounds may be of greater toxicological relevance in the lake. As anthropogenic influences continue to increase, SPMD-based sampling is expected to play a central role in future research concerned with the identification, monitoring and assessment of the risk posed by HOPs to Lake Shkodra/Skadar's aquatic biota. 相似文献
2.
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
3.
Zhu X Pfister G Henkelmann B Kotalik J Bernhöft S Fiedler S Schramm KW 《Environmental pollution (Barking, Essex : 1987)》2008,156(2):461-466
Gaseous emissions of combusted electronic scrap, PVC, carpet and wood were monitored for polycyclic aromatic hydrocarbons (PAHs) by simultaneous use of semipermeable membrane devices (SPMDs) and shoots of spruce needles (Picea abies). It was found that phenanthrene, acenaphthylene and fluorene were the dominating PAHs in all samples. SPMDs and needles mainly sequestered PAH associated with the vapor phase. Particle-bound PAHs were only detected in small amounts, at which the needles tended to uptake more of these compounds in comparison to the SPMDs. Nevertheless, the logarithm of the concentrations of PAHs analyzed in both passive samplers after the same sampling period exhibited a significant linear correlation with correlation coefficients larger than 0.8073. SPMDs and spruce needles can complement each other in passive air sampling for compounds with a preference to the gas phase rather than aerosols. 相似文献
4.
The effects of water flow rate and antifouling agents on the extent of biofouling and on the uptake of non-polar organic contaminants by semipermeable membrane devices (SPMDs) were studied during four field experiments in the Western Wadden Sea. Biofouling densities on the sampler surface ranged from 0.3 to 16 g dry weight dm−2. Water sampling rates were estimated from the dissipation rates of performance reference compounds (PRCs). The antifouling agents Irgarol and capsaicin (33 mg per ml triolein) had no noticeable effect on the extent of fouling, and caused only a 5–10% increase in the absorbed amounts. Enhanced flow rates had only a minimal effect on the amount of biofouling, but caused the water sampling rates to increase by a factor of 1.2–2. Increases in PRC-derived sampling rates were reflected by increases in the absorbed amounts for compounds that were in the linear uptake stage of the sampling process. The results imply (1) that extreme biofouling does not always result in reduced sampling rates, (2) that extreme biofouling does not preclude the existence of flow effects on the sampling rates, and (3) that differences in uptake rates are quantitatively reflected by the dissipation rates of PRCs. 相似文献
5.
利用半透膜被动采样技术监测黄河兰州段典型有机污染物 总被引:1,自引:0,他引:1
利用半透膜被动采样技术(SPMD)和固相萃取技术(SPE)对黄河兰州段八盘峡、包兰桥等六个监测断面的几种典型多环芳烃(PAHs)和壬基酚类(NPs)物质进行了采集测定。结果显示所选取的几种目标污染物在各监测点均有不同程度的检出。其中,几种PAHs在监测点水样中SPE测定的浓度为0.04~21.57g·L-1,而在SPMD中的浓度为842~99139g·L-1,富集倍数达到了103~105;NPs在监测点水样中SPE测定的浓度为0.04~2.10g·L-1,在SPMD中的浓度为80-81394g·L-1,富集倍数达到了103~104。利用SPMD数学模型,根据污染物在SPMD类酯中浓度推算出的污染物在水体中的平均浓度值,和利用SPE测得的水样中污染物的实际浓度值具有较高的相关性。该实验研究为发展SPMD技术作为黄河中有机污染物的常规监测手段提供一定的理论依据。 相似文献
6.
Gilli G Schilirò T Pignata C Traversi D Carraro E Baiocchi C Aigotti R Giacosa D Fea E 《Chemosphere》2005,61(11):1691-1699
Semipermeable membrane devices (SPMDs) mimic passive diffusive transport of bioavailable hydrophobic organic compounds through biological membranes and their partitioning between lipids and environmental levels. Our study was developed on a surface water treatment plant based in Turin, Northern Italy. The investigated plant treats Po River surface water and it supplies about 20% of the drinking water required by Turin city (about one million inhabitants). Surface water (input) and drinking water (output) were monitored with SPMDs from October 2001 to January 2004, over a period of 30 days. The contaminant residues, monthly extracted from SPMDs by dialysis in organic solvent, were tested with the MicrotoxTM acute toxic test and with the Ames mutagenicity test. Same extracts were also analyzed with gaschromatography—mass spectrometry technique in order to characterise the organic pollutants sampled, especially Polycyclic Aromatic Hydrocarbons (PAHs).
Although the PAHs mean concentration is about one hundred times lower in the output samples, the mean toxic units are similar in drinking and surface water.
Our data indicate that the SPMD is a suitable tool to assess the possible toxicity in drinking water. 相似文献
7.
Sirpa Herve Harry F. Prest Pertti Heinonen Tarja Hyötyläinen Jaana Koistinen Jaakko Paasivirta 《Environmental science and pollution research international》1995,2(1):24-30
Semipermeable membrane sampling devices (SPMDs) and caged lake mussels (Anodonta piscinalis) were simultaneously deployed at four lake watercourse sites in Central Finland four weeks in August 1992. This study was
part of the regular annual monitoring of the organochlorine compounds (OCC) in pulp-mill recipient watercourses of Finland
with bivalves. Chlorohydrocarbons (CHCs), chlorophenol compounds (PCPs), chloroanisoles (PCAs) and chloroveratroles (PCVs)
were analyzed from lipid extract of mussels and from the synthetic triolein lipid of the SPMDs. Hexane-diethyl ether (9:1,
v/v) dialysis using polyethylene membrane was applied in dean up of the SPMD lipids and, for comparison, to six sets of the
mussel fat. Dialysis recovered CHCs but not PCPs from the mussel fat. CHCs, PCPs, PCAs and PCVs were all recovered in dialysis
of the SPMD lipid. Handling of SPMDs in the transport and deployment operations caused significant OCC contamination for the
blank SPMDs. Similar trends were revealed in the OCC profiles for mussels ans SPMDs. An exception was the lack of PCPs appearing
in SPMDs that did appear in mussels and in a complementary manner the appearance of the PCAs and PCVs in SPMDs. 相似文献
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