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1.
Wu WZ  Schramm KW  Kettrup A 《Water research》2001,35(5):1141-1148
Bioaccumulation of PCDD/F in the foodweb was investigated in the Ya-Er Lake area, which was heavily polluted by PCDD/F. The high concentrations of PCDD/F in sediment can be transferred and bioaccumulated by aquatic organisms and humans through various pathways. Benthonic invertebrate animals and aquatic plants with a lot of fibers in the root can accumulate PCDD/F from sediment and water. Snail (Bellamya aeruginosa), shrimp (Macrobranchium sp.) and freshwater mussel (Acuticosta chinensis (Lea)) took up PCDD/F from the water and maintained the emission patterns, whereas fish tended to selectively accumulate 2,3,7,8-substituted isomers. The tissues of fish-eating bird and duck (Anas platyrhynchos) were very highly contaminated by PCDD/F due to ingestion of fish and other aquatic organisms from sediment. The residual concentration in breast milk depended on the original concentration of PCDD/F in the food. A resident in Ya-Er Lake area showed a daily intake of PCDD/F of about 9.14 pg TEQ/kg body weight/day. This is higher than the tolerable daily intake (TDI) for PCDD/F (1 pg TEQ/kg body weight/day), which was recommended by the World Health Organization (WHO).  相似文献   

2.
Two annually laminated cores collected from Lake DV09 on Devon Island in May 1999 were dated using 210Pb and 137Cs, and analyzed for a variety of halogenated organic contaminants (HOCs), including polychlorinated biphenyls (PCBs), organochlorine pesticides, short-chain polychlorinated n-alkanes (sPCAs), polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), and polybrominated diphenyl ethers (PBDEs). Dry weight HOC concentrations in Lake DV09 sediments were generally similar to other remote Arctic lakes. Maximum HOC fluxes often agreed well with production maxima, although many compound groups exhibited maxima at or near the sediment surface, much later than peak production. The lower than expected HOC concentrations in older sediment slices may be due to anaerobic degradation and possibly to dilution resulting from a temporary increase in sedimentation rate observed between the mid-1960s and 1970s. Indeed, temporal trends were more readily apparent for those compound classes when anaerobic metabolites were also analyzed, such as for DDT and toxaphene. However, it is postulated here for the first time that the maximum or increasing HOC surface fluxes observed for many of the major compound classes in DV09 sediments may be influenced by climate variation and the resulting increase in algal primary productivity which could drive an increasing rate of HOC scavenging from the water column. Both the fraction (F(TC)) and enantiomer fraction (EF) of trans-chlordane (TC) decreased significantly between 1957 and 1997, suggesting that recent inputs to the lake are from weathered chlordane sources. PCDD/Fs showed a change in sources from pentachlorophenol (PeCP) in the 1950s and 1960s to combustion sources into the 1990s. Improvements in combustion technology may be responsible for the reducing the proportion of TCDF relative to OCDD in the most recent slice.  相似文献   

3.
Animal agriculture in watersheds produces manure bacteria that may contaminate surface waters and put public health at risk. We measured fecal indicator bacteria (commensal Escherichia coli and fecal enterococci) and manure pathogens (Salmonella and E. coli 0157:H7), and physical-chemical parameters in pond inflow, within pond, pond outflow, and pond sediments in three ponds in agricultural watersheds. Bishop Pond with perennial inflow and outflow is located in the Piedmont, and Ponds A and C with ephemeral inflow and outflow in the Coastal Plain of Georgia. Bromide and chloride tracer experiments at Bishop Pond reflected a residence time much greater than that estimated by two models, and indicated that complete mixing within Bishop Pond was never obtained. The long residence time meant that fecal bacteria were exposed to solar UV-radiation and microbial predation. At Bishop Pond outflow concentrations of fecal indicator bacteria were significantly less than inflow concentrations; such was not observed at Ponds A and C. Both Salmonella and E. coli 0157:H7 were measured when concomitant concentrations of commensal E. coli were below the criterion for surface water impairment indicating problems with the effectiveness of indicator organisms. Bishop Pond improved down stream water quality; whereas, Ponds A and C with ephemeral inflow and outflow and possibly greater nutrient concentrations within the two ponds appeared to be less effective in improving down stream water quality.  相似文献   

4.
The development and application of a predictive fate model (DIG--Dioxins in Grenland) for polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/F) in the marine environment of the Norwegian Grenland Fjords are described. The objective of the modelling study was to predict long-term future changes in PCDD/F concentrations in the fjord following the cessation of point source emissions. To assess the reliability of the model, the model performance was evaluated by comparing model results to field measurements collected between 1989 and 2001. Model bias (defined as the ratio of median predicted concentration and median observed concentration) for prediction of concentrations for three different PCDD/F congeners (2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD), 1,2,3,6,7,8-hexadibenzofuran (HxCDF) and octachlorodibenzofuran (OCDF)) in the fjord was between 0.53 and 24, which was deemed a satisfactory result for models of this type. The model was run to determine the dynamic change in concentrations between 1950 and 2050 and to examine the key fluxes of PCDD/Fs in the fjord. Between 1990 and 2050 sediment concentrations of TCDD, HxCDF and OCDF were predicted to fall at fairly constant but gradually slowing rates to concentrations 52, 98 and 88 times lower, respectively, of their 1990 values. Losses of PCDD/Fs from the bottom sediments in the Frierfjord were predicted to be a combination of sediment burial and net resuspension to the water column. Sediment burial was shown to be relatively more important in the fjord's deep-water sediments, whereas resuspension was relatively more important in the shallow sediments. For the shallower sediments, a net water-to-sediment flux was predicted for all three congeners up until the mid-1970s, when emission reductions were initiated, and thereafter a net sediment-to-water flux was predicted. The shallow sediments acted as net sources to the deeper sediments and to the fishing areas in the outer fjord.  相似文献   

5.
The contamination of the Baltic Sea with polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) has resulted in restrictions on the marketing and consumption of Baltic Sea fish, making this a priority environmental issue in the European Union. To date there is no consensus on the relative importance of different sources of PCDD/Fs to the Baltic Sea, and hence no consensus on how to address this issue. In this work we synthesized the available information to create a PCDD/F budget for the Baltic Sea, focusing on the two largest basins, the Bothnian Sea and the Baltic Proper. The non-steady state multimedia fate and transport model POPCYCLING-Baltic was employed, using recent data for PCDD/F concentrations in air and sediment as boundary conditions. The PCDD/F concentrations in water predicted by the model were in good agreement with recent measurements. The budget demonstrated that atmospheric deposition was the dominant source of PCDD/Fs to the basins as a whole. This conclusion was supported by a statistical comparison of the PCDD/F congener patterns in surface sediments from accumulation bottoms with the patterns in ambient air, bulk atmospheric deposition, and a range of potential industrial sources. Prospective model simulations indicated that the PCDD/F concentrations in the water column will continue to decrease in the coming years due to the slow response of the Baltic Sea system to falling PCDD/F inputs in the last decades, but that the decrease would be more pronounced if ambient air concentrations were to drop further in the future, for instance as a result of reduced emissions. The study illustrates the usefulness of using monitoring data and multimedia models in an integrated fashion to address complex organic contaminant issues.  相似文献   

6.
Sewage contamination in shallow lake sediments is of concern because the pathogens, organic matter and nutrients contribute to the deterioration of the water-bodies' health and ecology. Sediment cores from three shallow lakes (Coneries, Church and Clifton Ponds) within Attenborough nature reserve located downstream of sewage treatment works were analysed for TOC, C/N, δ13C, δ15N, bacterial coliforms and faecal sterols. 210Pb and 137Cs activities were used to date the sediments. Elemental analysis suggests that the source of organic matter was algal and down profile changes in δ13C indicate a possible decrease in productivity with time which could be due to improvements in sewage treatment. δ15N for Coneries Pond are slightly higher than those observed in Church or Clifton and are consistent with a sewage-derived nitrate source which has been diluted by non-sewage sources of N. The similarity in δ15N values (+ 12‰ to + 10‰) indicates that the three ponds were not entirely hydrologically isolated. Analysis by gas chromatography/mass spectrometry (GC/MS) reveals that Coneries Pond had sterol concentrations in the range 20 to 30 μg/g (dry wt.), whereas, those from Clifton and Church Ponds were lower. The highest concentrations of the human-sourced sewage marker 5β-coprostanol were observed in the top 40 cm of Coneries Pond with values up to 2.2 μg/g. In contrast, Church and Clifton Pond sediments contain only trace amounts throughout. Down-profile comparison of 5β-coprostanol/cholesterol, 5β-coprostanol/(5β-coprostanol + 5α-cholestanol) and 5β-epicoprostanol/coprostanol as well as 5α-cholestanol/cholesterol suggests that Coneries Pond has received appreciable amounts of faecal contamination. Examination of 5β-stigmastanol (marker for herbivorous/ruminant animals) down core concentrations suggests a recent decrease in manure slurry input to Coneries Pond. The greater concentration of β-sitosterol in sediments from Church and Clifton Ponds as compared to Coneries is attributed in part to their greater diversity and extent of aquatic plants and avian faeces.  相似文献   

7.
The partitioning behaviour of the organic biocides, Irgarol 1051 and diuron and two inorganic biocides (copper and zinc) was investigated using six sediments of differing physico-chemical properties collected from unimpacted sites along the south coast of England. The kinetics of sorption and equilibrium partitioning between the sediments and seawater were investigated over a period of 20 days. Resulting organic carbon/water partition coefficients (log Koc) were related to suspended sediment concentration and ranged from 2.28 to 5.20 for diuron; and from 2.41 to 4.89 for Irgarol 1051. Sediment/water partition coefficients (log Kp) for copper and zinc varied from 2.46 to 5.08 l/kg and from 2.49 to 4.97 l/kg, respectively. Kinetic data indicated that there were significant interactions between the dissolved and particulate phases at the start of the experiments, just after mixing. This is thought to be a result of redistribution of organic carbon between the two phases.  相似文献   

8.
In spring 2006, an Asian dust storm (ADS) that originated in the deserts of Mongolia and China eventually reached populated areas of East Asia, including Taiwan. The concentrations of total suspended particles (TSP), vapor/solid-phase dioxin-like compounds and metal content in atmospheric aerosols were monitored at two sampling sites in northern Taiwan during the ADS episode: one along the northern coast (Site A), and the other in Taipei city (Site B). The ADS swept across northern Taiwan from 13 March to 19 March, 2006. Data indicate that the atmospheric dibenzo-p-dioxin and dibenzofuran (PCDD/F, 32.2 to 52.5 fg-I-TEQ/m(3)) and polychlorinated biphenyl (PCB, 2.23 to 4.49 fg-TEQ(WHO)/m(3)) concentrations measured at the two sampling sites prior to the ADS episode were considerably lower than those measured in other Asian countries. However, measurements made at both sites on 13 and 18 March 2006 indicate that the atmospheric PCDD/F and PCB concentrations increased 2.5 and 3.2 times at Site A, and 2.1 and 1.9 times at Site B, respectively, during the ADS episode. The concentrations of aluminum (Al), potassium (K) and Titanium (Ti) in atmospheric aerosols were also found to increase about 2 to 5 times during this period. As no specific dioxin emission sources exist within nearly 20 km of Site A, the increase in PCDD/F and PCB concentrations observed there is likely to be related to the ADS from mainland China. Additionally, the amount of PCDD/Fs bound to suspended particles increased from 257-259 to 339-512 pg-I-TEQ/g-TSP during the ADS episode. The distribution of OCDD congener observed in Taipei city increased dramatically during the ADS episode, however, the distribution of PCB congener did not vary significantly.  相似文献   

9.
Phosphorus (P) may be liberated from lake sediments by reductive dissolution of Fe(OH)(3(S)) during periods of hypolimnetic anoxia. P, however, remains adsorbed to Al(OH)(3(S)) regardless of redox conditions. During chronic or episodic acidification of a catchment, ionic Al is mobilized from soils to receiving waters. A fraction of the mobilized Al may precipitate as a consequence of higher pH of the receiving waters. We hypothesized that phosphorus retention in lake sediments is directly related to the magnitude of Al loading in response to low pH in the watershed. We studied cores representing over 200 years of sediment accumulation in historically acidic Mud Pond and Little Long Pond in eastern Maine, USA. Sequential chemical extractions of sediment were used to assess the history of Al, Fe, and P interactions. Mud Pond is a first-order pond with a pH of approximately 4.7, having acidified slightly in response to anthropogenic acidification from approximately 1930. The inlet stream to Mud Pond has dissolved Al concentrations often exceeding 500 microg/L, of which more than half is organically-bound. Mud Pond drains into Little Long Pond, a second-order pond with a historical pH of <6, and which has shown little pH or alkalinity response to increases or decreases in atmospheric SO(4)(2-) input. Sequential extractions show that Al and P are predominantly in the 0.1 M NaOH-extractable fraction in the sediments from both ponds throughout the cores. The concentration of the likely biogenic and non-reactive P within the NaOH fraction increases up core from <30% to approximately 60%. Extractable Fe (<20% of extractable Al) is mainly in the 0.1 M NaOH-extractable fraction, except for the top few cm, which are predominantly in the bicarbonate-dithionite reducible fraction. Accumulation rates of sediment, Al, Fe, and P in both ponds have increased in the last 50-60 yr, but fractions remain in the same proportion. Throughout both sediment cores the molar ratio of specific Al:P fractions greatly exceeds 25, and molar ratio of specific Al:Fe fractions greatly exceeds 3, the thresholds proposed by Kopácek et al. [Kopácek J, Borovec J, Hejzlar J, Ulrich K-U, Norton SA, Amirbahman A. Aluminum control of phosphorus sorption by lake sediments. Environ Sci Technol 2005; 39: 8784-89.] for P release during anoxia. The data illustrate a continuous association of P with Al in both ponds during the last two centuries, likely due to the persistent natural acidity of the catchments.  相似文献   

10.
Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) are persistent organic pollutants that are resistant to environmental and biological degradation and disperse into various environmental compartments throughout the atmosphere, water, soil, sediments, and food. Many factors, such as age, sex, lifestyle, and metabolism, can explain the distribution of serum levels after humans exposed to PCDD/Fs. The aim of our study was therefore to investigate the PCDD/Fs distribution and profile of the general population in northern Taiwan. All selected subjects were between 18 and 65 years old and proportionally chosen from five age groups based on population distribution of each district or county. Higher serum PCDD/F levels were found in the elder than in the young, and in females than in males. In addition, nonsmokers and passive smokers showed higher levels of PCDD/Fs than active smokers. The serum concentrations of 2,3,4,7,8-PeCDF; 1,2,3,7,8-PeCDD; and 1,2,3,6,7,8-HxCDD in some subjects seemed to increase with their age, which might have been caused by the longer half-lives of these substances. In future studies, more information about food consumption, occupational exposure, open-combustion, and other potential factors needs to be collected to clarify the most important factors affecting the distribution of serum PCDD/Fs in the general population in Taiwan.  相似文献   

11.
E Eljarrat  J Caixach  J Rivera 《Water research》2001,35(11):2799-2803
The fate of polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) in sewage sludges after discharge into the sea was investigated. Sediment samples were analysed at a sewage sludge disposal site as well as in the surrounding areas. Moreover, eight sediment samples from two rivers in Catalonia and three sediment samples from Catalonian Coast were analysed to determine the background levels of contamination. Total international toxicity equivalent (I-TEQ) values for these sediments ranged from 0.42 to 8.01 pg g, with a mean value of 4.15 pg/g and a median value of 3.69 pg/g. However, the I-TEQ values of sludge-treated areas were higher: 57.04 pg/g at the dumping site, and within a range of 13.42-47.76 pg/g near this site. Thus, European sediment quality objectives were exceeded. The higher concentrations coincided with changes in the ratio between PCDD and PCDF levels, suggesting the influence of the sewage sludge on coastal sediments.  相似文献   

12.
Analysis of blood samples is an effective way of evaluating contamination by persistent pollutants such as polybrominated diphenyl ethers (PBDEs), polychlorinated dibenzo-p-dioxin/furans (PCDD/Fs), and polychlorinated biphenyls (PCBs) in human population. Concentrations of PBDEs, PCDD/Fs and PCBs were measured in the blood of laborers (n = 13) working full time in two different municipal waste incinerator (MWI) plants and residents from the general population (n = 22) living in areas near MWIs in Korea. The concentrations of PBDEs were found to be slightly higher in the blood of incineration workers (8.61-46.05 ng/g lipid; mean, 19.33 ng/g lipid; median, 15.94 ng/g lipid) in comparison to that of residents from the general population (7.24-28.89 ng/g lipid; mean, 15.06 ng/g lipid; median, 14.34 ng/g lipid). The total average PCDD/Fs and PCB TEQ concentration was 20.11 pg/g lipid, averaged over incineration workers (17.73 pg/g lipid) and the general population (21.52 pg/g lipid). In addition, the average total crude concentration of PCDD/Fs was 7.40 ng/g lipids, which was 4.1 times greater than for PBDEs. Congener specific analysis confirmed that BDE 47 was a predictive indicator for total PBDE concentration (correlation coefficient r = 0.912), and that PCB 153 was a predictive indicator for total PCB concentration (r = 0.967). The PBDE levels in human blood in Korea are much higher than those reported in other countries. The presence of the BDE 183 congener was characteristic in the blood of workers from an electronic dismantling facility in MWIs.  相似文献   

13.
Chen B  Xuan X  Zhu L  Wang J  Gao Y  Yang K  Shen X  Lou B 《Water research》2004,38(16):3558-3568
Ten polycyclic aromatic hydrocarbons (PAHs) were simultaneously measured in 17 surface water samples and 11 sediments of four water bodies, and 3 soils near the water-body bank in Hangzhou, China in December 2002. It was observed that the sum of PAHs concentrations ranged from 0.989 to 9.663 microg/L in surface waters, from 132.7 to 7343 ng/g dry weight in sediments, and from 59.71 to 615.8 ng/g dry weight in soils. The composition pattern of PAHs by ring size in water, sediment and soil were surveyed. Three-ring PAHs were dominated in surface waters and soils, meanwhile sediments were mostly dominated by four-ring PAHs. Furthermore, PAHs apparent distribution coefficients (K(d)) and solid f(oc)-normalized K(d) (e.g. K(oc)= K(d) / f(oc)) were calculated. The relationship between logK(oc) and logK(ow) of PAHs for field data on sediments and predicted values were compared. The sources of PAHs in different water bodies were evaluated by comparison of K (oc) values in sediments of the river downstream with that in soils. Hangzhou section of the Great Canal was heavily polluted by PAHs released from industrial wastewater in the past and now PAHs in sediment may serve as sources of PAHs in surface water. PAHs in Qiantang River were contributed from soil runoff. Municipal road runoff was mostly contributed to West Lake PAHs.  相似文献   

14.
Contaminated sediments pose a unique challenge for risk assessment or remediation because the overlying water column may transport contaminants offsite or to ecological receptors. This research compares the behavior of polycyclic aromatic hydrocarbons (PAHs) on marine sediments from two sites. The first site was affected by shipping activities and the second was impacted by a creosote seep. Organic carbon:water partitioning coefficients (Koc values) were measured with three solutions. Desorption was measured using Tenax beads. PAHs from the ship channel had lower Koc values than those from the creosote facility. For example, the average logKoc value of ship channel pyrene was significantly lower than that of creosote facility pyrene (4.39 +/- 0.35 and 5.29 +/- 0.09, respectively, when tested in 5 mM calcium chloride). These results were consistent with the greater desorption of pyrene, phenanthrene and benzo(a)pyrene from the ship channel than from the creosote facility sediments. Organic compound desorption from sediments can be considered to be a two-stage process, with a labile fraction that desorbs quickly and a refractory fraction that desorbs much more slowly. In both sediments, more than 75% of the benzo(a)pyrene was found to have partitioned into the refractory phase. The amounts of phenanthrene and pyrene that partitioned into the refractory phase were lower. Linear correlations of logKoc with log(CR/CL) (where CR and CL are the fractions of the compound in the refractory and labile phases, respectively, at time zero) showed that partitioning measurements made with the US EPA's Toxicity Characteristic Leaching Procedure fluid (US EPA, 1996) most closely matched predictions of desorption behavior. The data imply that with a larger data set, it may be possible to relate simple partitioning measurements to desorption behavior. Partitioning measurements were used to predict water concentrations. Despite having higher concentrations of carcinogenic PAHs [cPAHs, the seven PAHs categorized by the US EPA (2004) as class B2 carcinogens], creosote facility sediments were predicted to produce lower aqueous concentrations of cPAHs. These results indicate that both sediment and contaminant characteristics will impact contaminant release from sediments.  相似文献   

15.
Mary Lake, St. George Lake, and Philips Lake are located in the Greater Toronto Area, Ontario, Canada. These lakes are relatively small and have no direct inflow and outflow channels. Mercury (Hg) input to the lakes comes mainly from atmospheric deposition. Sediment cores from the points of the maximum lake depth and surface sediment samples from the points of maximum lake depth to the bank of each lake were collected in October 2005. Total and methyl mercury concentrations in the pore water and sediments of these samples were determined. In these small lakes with high organic content, there was no correlation between organic content and total mercury (THg) in the samples throughout the entire sediment cores while strong positive correlation between these two parameters was observed in all the surface sediments. Compared with typical methylmercury (MeHg) depth-profiles of sediment cores in other studies, where MeHg concentrations and methylation rates decreased sharply with increasing depth, MeHg distributions in the sediment cores in this study showed that MeHg might have been produced not only in the upper sediment but also in the deeper sediments, which resulted in a larger MeHg reservoir in the sediment. Organic matter, to some extent, affected MeHg distributions in the samples throughout the entire sediment cores. Concentrations of MeHg in all the surface sediments, however, were not controlled by organic matter, whereas they were largely a function of water column depths. Total mercury concentrations in pore water were relatively homogenous in both the sediment cores and surface sediment while MeHg in pore water generally deceased with increasing depth in the sediment cores and increasing distance from the centre of the lakes in surface sediments. Methylmercury contributed 1% to 76% of THg in the pore water samples. Concentrations and distributions of MeHg in overlying water and sediment-surface water in Mary Lake and St. George Lake suggested that both in situ production of MeHg in lake water and the release of MeHg from sediment contributed to high MeHg in deep anoxic water.  相似文献   

16.
Forest fires are believed to produce polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs); however, there is no firm evidence supporting this conjecture. To address this issue, we investigated whether PCDD/Fs and polycyclic aromatic hydrocarbons (PAHs) are formed by forest fires. The present work takes the indirect approach of measuring the levels of PCDD/Fs and PAHs in soil and ash samples 1, 5 and 9 months after forest fires. To determine if PCDD/Fs or PAHs were formed during forest fires, the levels of PCDD/Fs and PAHs measured in the burnt soil samples were compared with those in the corresponding unburnt soil samples. One month after forest fires, the concentrations of PCDD/Fs and PAHs in burnt soils were higher than in the corresponding unburnt soils. In addition, the homologue profiles differed between the burnt and unburnt soils. Five months after forest fires, however, the concentrations of PCDD/Fs and PAHs in the burnt soils were similar to those in unburnt soils. The data presented here strongly suggest that PCDD/Fs and PAHs form during forest fires and are then introduced into the soil. The results further suggest that the ash resulting from the combustion of wood and other organic matter is the main agent influencing the concentration of PCDD/Fs and PAHs in the soil.  相似文献   

17.
A comprehensive sampling program was conducted at four sampling sites in the vicinity area of a Waelz plant prior to and after the retrofitting of this plant for reducing PCDD/F (polychlorinated dibenzo-p-dioxin and polychlorinated dibenzofuran) and polychlorinated biphenyl (PCB) emission to evaluate its effects on atmospheric PCDD/F and PCB concentrations. During the shutdown stage of the Waelz plant investigated, the atmospheric PCDD/F and PCB concentrations measured in the vicinity area (sites A, B and C) range from 24 to 170 fg-I-TEQ/m(3) and 5.0 to 8.2 fg-TEQ(WHO)/m(3), respectively. As the facility restarted to operate, the atmospheric PCDD/F and PCB concentrations measured increased to 570-1460 fg-I-TEQ/m(3) and 23-59 fg-TEQ(WHO)/m(3), respectively. When activated carbon injection (ACI) was adopted in the facility in early 2006, the PCDD/F concentrations measured in stack gas decreased dramatically from 190 to 3.4 ng-I-TEQ/Nm(3), while the PCB concentrations decreased from 4.9 to 0.08 ng-TEQ(WHO)/Nm(3). In the meantime, the atmospheric PCDD/F and PCB concentrations measured at sites A, B and C decreased to 150-340 fg-I-TEQ/m(3) and 13-19 fg-TEQ(WHO)/m(3), respectively. However, relatively high PCDD/F (180-1460 fg-I-TEQ/m(3)) and PCB (9.3-59 fg-TEQ(WHO)/m(3)) concentrations were measured at site D during all sampling stages. Overall, atmospheric sampling results indicate that over 50% of PCDD/Fs distributed in solid phase, while over 90% of PCBs distributed in vapor phase during all sampling stages.  相似文献   

18.
This paper investigated the effect of inorganic chlorine on the formation of PCDD/Fs from heating polyethylene (PE) in the presence of air. There was an increase in the formation of PCDD/Fs with an increasing amount of metal chlorides except NaCl, which was not observed to have any effects on the formation of PCDD/Fs without the presence of catalysts. Although the levels of PCDD/Fs formation in this study have no relevance to full scale municipal solid waste incineration, the results of the present experiments can aid understanding of the mechanisms of the formation of PCDD/Fs from heating PE in the presence of metal chlorides.  相似文献   

19.
Polychlorinated dibenzo-p-dioxins (PCDDs) and -furans (PCDFs) are ubiquitous in the environment. This paper estimates the present UK environmental loading of PCDD/Fs in soils, vegetation, air, water and sediments. Greater than 95% of the estimated total PCDD/F loading of 5.7 t in the UK environment is present in surface soils. Annual emissions from known primary sources of PCDDs and PCDFs are estimated. The most important of these include: municipal waste incinerator stack emissions (10.9 kg sigma PCDD/F per annum); industrial (7.7 kg/year) and domestic (5.1 kg/year) combustion of coal; clinical waste incinerators (1.7 kg/year); volatilisation from chlorophenol-treated substrates (1.7 kg/year) and combustion of leaded petrol by motor vehicles (0.7 kg/year). These sources are generally easy to define and reasonably reliable national estimates can be obtained. More difficult to quantify are secondary releases from the large UK stock of pentachlorophenol (PCP) and PCP-treated products, which may represent quantitatively one of the most important sources of total PCDD/Fs to the environment. Estimates of homologue-specific emissions indicate that combustion processes represent a far more significant source of tetra and penta CDD/Fs than do chlorophenols, which in turn constitute a greater source of hepta- and octachlorinated congeners. Direct emission of PCDD/Fs into the atmosphere from combustion processes facilitates their atmospheric transport to remote locations. This, coupled with the diffuse nature of combustion processes, means that the effects of PCDD/F contamination originating from anthropogenic combustion are more widespread than those from the use and disposal of chlorophenols. Contamination from chlorophenols will be more localised, owing to the insignificance of direct atmospheric release pathways for this source. Although there is reasonable agreement between the estimated current annual flux and the present UK environmental loading of PCDDs and PCDFs, a large discrepancy exists between the sum of the annual contributions from primary sources and this annual flux. Whilst the existence of an as yet unidentified source or sources or gross underestimates of known sources cannot be excluded, it is proposed that much of this discrepancy may be accounted for by secondary releases from the use and disposal of chlorophenols and the long-range transport, continued remobilisation and subsequent redeposition of PCDDs and PCDFs already present in the environment. Despite limited evidence for a modest decline in levels of PCDDs and PCDFs in some environmental compartments over the last 20 years, the environmental persistence of these chemicals means that they will remain in the UK environment for the foreseeable future despite recent action to curb primary emissions.  相似文献   

20.
This paper discusses the dioxin TEQ levels as determined by the chemically activated luciferase gene expression assay (CALUX) and by HRGC-HRMS in eggs, soils, faeces and kitchen waste samples obtained in the CONTEGG study. The samples were collected in each Belgian province at private homes and in small gardens where chickens are held. The CALUX levels for eggs sampled in autumn were higher than the levels in eggs obtained at the same locations in spring (median values of 5.86 and 4.08 pg CALUX TEQ/g fat, respectively). The total WHO-TEQ levels in eggs, determined by HRGC-HRMS, ranged from 3.29 to 95.35 pg TEQ/g fat in autumn and from 1.50 to 64.79 pg TEQ/g fat in spring. In the soils on which the chickens forage, levels of 2.51-11.35 pg I-TEQ/g in autumn and 2.00-7.86 pg I-TEQ/g in spring were found. The congener pattern of PCDD/Fs in the eggs, soils and faeces was dominated by OCDD, in addition to 1,2,3,4,6,7,8-HeptaCDD, OCDF and 1,2,3,4,6,7,8-HeptaCDF. The predominant dioxin-like PCBs were PCB118, PCB 105 and PCB 156. The dioxin-like PCBs contributed on average 47%, 14% and 20% to the total WHO-TEQ in eggs, soils and faeces, respectively. Kitchen waste samples were very low-contaminated with dioxin-like compounds. The present results showed a good agreement between egg and soil TEQ levels for PCDD/Fs but not for dioxin-like PCBs. This study showed that current soil levels found in some private gardens do not lead to egg levels below the current EU maximal level of 6 pg total TEQ/g fat for dioxins and dioxin-like PCBs. The consumers of the analysed eggs attained 5-79% of the tolerable weekly intake (TWI) of 14 pg TEQ/kg bw for dioxins and dioxin-like PCBs by exposure to their home-produced eggs only.  相似文献   

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