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1.

Background  

Export to the deep sea has been found to be a relevant pathway for highly hydrophobic chemicals. The objective of this study is to investigate the influence of this process on the potential for long-range transport (LRT) of such chemicals.  相似文献   

2.
The long-range transport of persistent organic pollutants (POPs) is investigated with two multimedia box models of the global system. ChemRange is a purely evaluative, one-dimensional steady-state (level III) model; CliMoChem is a two-dimensional model with different temperatures, land/water ratios and vegetation types in different latitudinal zones. Model results are presented for three case studies: (i) the effect of atmospheric aerosol particles on the long-range transport of POPs, (ii) the effect of oceanic deposition on the long-range transport of different PCB congeners, (iii) the global fractionation of different PCB congeners. The model results for these case studies show: (i) the low atmospheric half-lives estimated for several organochlorine pesticides are likely to be inconsistent with the observed long-range transport of these compounds; (ii) export to the deep sea reduces the potential for long-range transport of highly hydrophobic compounds (but does not remove these chemicals from the biosphere); (iii) there are different meanings of the term global fractionation that refer to different aspects of the fractionation process and need to be distinguished. The case-study results further indicate that the influences of varying environmental conditions on the physicochemical properties and the degradation rate constants of POPs need to be determined.  相似文献   

3.
In the last years, the spatial range (SR) or characteristic travel distance (CTD) of organic chemicals has found increasing scientific interest as an indicator of the long-range transport (LRT) potential and, in combination with persistence, as a kind of 'hazard' indicator on the exposure level. This development coincides with European debates about more effective and more preventive approaches to the chemicals assessment, and about an international, legally-binding instrument for the phase out of persistent organic pollutants (POPs). Persistence and LRT potential are important issues in these debates. Here, the development of the concept of assessing the spatial scale from early ideas in the 1970s and 1980s to recent studies in the field of multimedia fate and transport modeling is summarized. Different approaches to the modeling of environmental transport (advective and dispersive) and different methods for quantifying the SR or CTD are compared. Relationships between SR or CTD and different persistence measures are analyzed. Comparison of these relationships shows that conclusions for chemical assessment should be based on an evaluation of different persistence and spatial scale measures. The use of SR or CTD and persistence as hazard indicators in the chemicals assessment is illustrated.  相似文献   

4.
Background, Aim and Scope Modelling of the fate of environmental chemicals can be done by relatively simple multi-media box models or using complex atmospheric transport models. It was the aim of this work to compare the results obtained for both types of models using a small set of non-ionic and non-polar or moderately polar organic chemicals, known to be distributed over long distances. Materials and Methods Predictions of multimedia exposure models of different types, namely three multimedia mass-balance box models (MBMs), two in the steady state and one in the non-steady state mode, and one non-steady state multicompartment chemistry-atmospheric transport model (MCTM), are compared for the first time. The models used are SimpleBox, Chemrange, the MPI-MBM and the MPI-MCTM. The target parameters addressed are compartmental distributions (i.e. mass fractions in the compartments), overall environmental residence time (i.e. overall persistence and eventually including other final sinks, such as loss to the deep sea) and a measure for the long-range transport potential. These are derived for atrazine, benz-[a]-pyrene, DDT, α and γ-hexachlorocyclohexane, methyl parathion and various modes of substance entry into the model world. Results and Discussion Compartmental distributions in steady state were compared. Steady state needed 2–10 years to be established in the MCTM. The highest fraction of the substances in air is predicted by the MCTM. Accordingly, the other models predict longer substance persistence in most cases. The results suggest that temperature affects the compartmental distribution more in the box models, while it is only one among many climate factors acting in the transport model. The representation of final sinks in the models, e.g. burial in the sediment, is key for model-based compartmental distribution and persistence predictions. There is a tendency of MBMs to overestimate substance sinks in air and to underestimate atmospheric transport velocity as a consequence of the neglection of the temporal and spatial variabilities of these parameters. Therefore, the long-range transport potential in air derived from MCTM simulations exceeds the one from Chemrange in most cases and least for substances which undergo slow degradation in air. Conclusions and Perspectives MBMs should be improved such as to ascertain that the significance of the atmosphere for the multicompartmental cycling is not systematically underestimated. Both types of models should be improved such as to cover degradation in air in the particle-bound state and transport via ocean currents. A detailed understanding of the deviations observed in this work and elsewhere should be gained and multimedia fate box models could then be ‘tuned in’ to match better the results of comprehensive multicompartmental transport models. ESS-Submission Editor: Prof. Dr. Michael Matthies (matthies@uos.de)  相似文献   

5.
A three-dimensional/high-resolution transport model for persistent organic pollutants (POPs) has been developed for the East China Sea (ECS). The POPs model has four compartments (gaseous, dissolved, phytoplankton-bound, and detritus-bound phases) and includes processes for diffusive air-water exchange, phytoplankton uptake/depuration to POPs, decomposition of dissolved phase, vertical sinking of phytoplankton, detritus production by phytoplankton mortality, and vertical sinking and decomposition of detritus. The POPs model is coupled with an ocean circulation model that can reproduce the seasonal variation in physical variables to represent the advection and diffusion of POPs. We applied the POPs model to the polychlorinated biphenyl congener 153 (PCB 153) from the atmosphere and examined the behavior of PCB 153 in the ocean. The model showed a remarkable seasonal variability of PCB 153. Concentrations in the dissolved and particulate phases are high in winter (January-March) and low in summer (July-September). In coastal regions, where chlorophyll a concentration is high, horizontal and vertical distributions in the dissolved and particulate PCB 153 concentrations are strongly affected by phytoplankton uptake. The sensitivity experiments on the dynamics of PCB 153 suggested that a change of Henry’s law constant associated with water temperature is the major factor controlling the seasonal variability of PCB 153. The model-based yearly mass balance of PCB 153 in the ECS indicated that most of the atmospheric input (35.5 kg year−1) is removed by the horizontal advection outside the ECS (19.0 kg year−1) and accumulates to the sea bottom by vertical sinking (15.7 kg year−1). For comparison with PCB 153, we also conducted simulations for PCB 52, 101, and 180. The seasonal variations are similar to that of PCB 153. The mass balance of PCB 52 that has short half-life time and less hydrophobic property shows the different results compared with PCB 101, 153, and 180.  相似文献   

6.
Continental-scale distribution and inter-continental transport of four polychlorinated biphenyl (PCB) congeners (28, 101, 153, 180) from 1950 to 2010 were studied using the global multicompartment chemistry transport model MPI-MCTM. Following identical primary emissions for all PCB congeners into air, most of the burden is stored in terrestrial (soil and vegetation) compartments. Thereby, PCB-28, PCB-101 and PCB-153 show a shift of the soil burden maxima from source to remote regions. This shift is downwind with regard to the westerlies for Eurasia and upwind for North America and more prominent for the lighter PCBs than for PCB-153 or PCB-180. In meridional direction, all congeners' distributions underwent a northward migration in Eurasia and North America since the 1950s. Inter-continental transport from Eurasian sources accounts largely for contamination of Alaska and British Columbia and determines the migration of the PCB distribution in soil in North America. Trans-Pacific transport occurs mainly in the gas phase in boreal winter (December-January-February) at 3-4 km altitude and is on a multi-year time scale strongly linked to the atmospheric pressure systems over the Pacific. Inter-continental transport of the lighter, more volatile PCBs is more efficient than for the heavier PCBs.  相似文献   

7.
The hazard indicators persistence (P) and long-range transport potential (LRTP) are used in chemicals assessment to characterize chemicals with regard to the temporal and spatial extent of their environmental exposure. They are often calculated based on the results of multimedia fate models. The environmental and substance-specific input parameters of such models are subject to a range of methodological uncertainties and also influenced by natural variability. We employed probabilistic uncertainty analysis to quantify variance in P and LRTP predictions for chemicals with different partitioning and transport behavior. Variance found in the results is so large that it prevents a clear distinction between chemicals. Additionally, only small improvements are observed when evaluating the results relative to a benchmark chemical. This can be explained by the dominance of substance-specific parameters and the only small direct influence of environmental parameters on P and LRTP as model outcomes. The findings underline the importance of learning how environmental conditions cause variability in substance behavior for improved substance ranking and classification.  相似文献   

8.
We present the Berkeley-Trent North American contaminant fate model (BETR North America), a regionally segmented multimedia contaminant fate model based on the fugacity concept. The model is built on a framework that links contaminant fate models of individual regions, and is generally applicable to large, spatially heterogeneous areas. The North American environment is modeled as 24 ecological regions, within each region contaminant fate is described using a 7 compartment multimedia fugacity model including a vertically segmented atmosphere, freshwater, freshwater sediment, soil, coastal water and vegetation compartments. Inter-regional transport of contaminants in the atmosphere, freshwater and coastal water is described using a database of hydrological and meteorological data compiled with Geographical Information Systems (GIS) techniques. Steady-state and dynamic solutions to the 168 mass balance equations that make up the linked model for North America are discussed, and an illustrative case study of toxaphene transport from the southern United States to the Great Lakes Basin is presented. Regionally segmented models such as BETR North America can provide a critical link between evaluative models of long-range transport potential and contaminant concentrations observed in remote regions. The continent-scale mass balance calculated by the model provides a sound basis for evaluating long-range transport potential of organic pollutants, and formulation of continent-scale management and regulatory strategies for chemicals.  相似文献   

9.
In 2006, levels of seven indicator polychlorinated biphenyl congeners (PCB28, 52, 101, 118, 138, 153, and 180) in blood serum of 202 blood donors residing for more than 2 years in five urban areas included in the Czech Human Biomonitoring project were measured by GC/MS/MS method. PCB congeners 138, 153 and 180 accounted for about 97% of the sum of the indicator congeners analyzed. Overall, the median and 95th percentile of the most abundant congener PCB 153 were 438 ng/g lipid and 1079 ng/g lipid, respectively. The highest median levels were found in Uherské Hradiste (669 ng/g lipid) and Ostrava (672 ng/g lipid in males compared to 341 ng/g lipid in females). Serum PCB concentrations were significantly associated with age, gender, place of residence and smoking habit, but not with body mass index and education. The results suggest the importance of PCB body burden in the Czech general population and the existence of hot spots.  相似文献   

10.
Data on dioxin-like PCB in indoor air of buildings with PCB-containing materials and on possible correlation between toxicity equivalent concentrations (TEQ) and levels of non-dioxin-like standard PCB is sparse. As part of a larger survey on indoor-air contamination with PCB, the connection between the concentration of standard PCB congeners and the dioxin-like toxicity expressed as TEQ was investigated. Indoor air samples (n=8) were collected in four public buildings with known PCB sources and total PCB levels in the range from 715 to 2250 ng/m3 and analyzed for the six non-dioxin-like standard PCB (congeners 28, 52, 101, 138, 153, 180), the twelve dioxin-like PCB congeners according to WHO and the 17 2,3,7,8-substituted PCDD/PCDF congeners. In three buildings where PCB were used as flame retardant coatings of acoustic ceiling tiles, PCB 101 had the maximum level among the six standard PCB, while in the building with permanent elastic sealants as PCB source, congeners 28 and 52 dominated the pattern by far. In the case of permanent elastic sealants as PCB source (n=3) a total PCB concentration of 1000 ng/m3 corresponded to a total TEQ level of 0.3-0.6 pg/m3. In contrast, in rooms with acoustic ceiling tiles as PCB source, 1.8-4.7 pg TEQ/m3 per 1000 ng total PCB/m3 were found. Linear regression analysis between PCB and TEQ indicated that PCB 118 might be used to calculate the total TEQ of dioxin-like PCB and PCDD/PCDF. By means of such a correlation it is possible to estimate TEQ by extrapolation from the results of less sophisticated analytical methods. It is tentatively recommended to use PCB 118 for screening purposes or re-evaluation of standard PCB indoor-air measurements. If only the six non-dioxin-like PCB standard congeners are available, a regression algorithm using the sum of PCB 101, 138, 153 and 180 might be used instead.  相似文献   

11.
In order to get more information about potential health hazards due to indoor air PCBs the present study investigated the PCB indoor concentration in schools as well as the blood levels of 6 PCB-indicator congeners in teachers from these schools. 151 teachers (78 male and 73 female; mean age 48 years) from 3 contaminated and 2 control schools participated in the study. Maximal indoor air values for total PCBs (6 PCB-indicator congeners times 5) in schools ranged from 1587 to 10655 ng/m3. Blood analyses indicated an increase in mean PCB 28 level from 0.036 (control group) to 0.098 microg/l in teachers from a school with heavy contamination of low chlorinated PCB. But there was no significant increase of PCB 138, 153 and 180 in blood above the normal background concentrations in any of the contaminated schools (mean values of all groups: PCB 138 = 0.66, 153 = 0.95, 180 = 0.70 microg/l blood). The results of blood analyses and additional toxicokinetic calculations suggested that inhalative PCB-uptake in the most contaminated schools caused a minor increase above mean background-PCB concentrations in blood. In conclusion, despite high PCB indoor air levels in schools, there was only a moderate increase in blood concentrations of teachers, mainly due to congeners with low chlorination (PCB 28 to PCB 101).  相似文献   

12.
13.
Climate change influence on POPs distribution and fate: a case study   总被引:2,自引:0,他引:2  
Climate change has the potential of affecting the behaviour and distribution of organic pollutants, including POPs. Direct effects of climate change, like temperature increase, modification of wind and precipitation patterns, sea level rise, snow and ice cover, may be very effective in altering the partitioning of POPs among the environmental compartments. Other consequences of future climate scenarios may imply the alteration of degradation rates, soil properties (and hence land use), air-particle partitioning of chemicals and so forth. A case study is here presented to illustrate the major implications of climate change on the long term at the local scale. A dynamic multimedia model was applied to selected PCB and PCDD/F congeners to simulate the effects of climate change on their distribution and fluxes over the next 50 y in the Venice Lagoon (Italy). Different climate change scenarios were tested, finding noticeable variations in POPs concentration even for minor environmental changes. PCBs and PCDFs environmental concentrations may differ by a factor two in a moderate climate change scenario, compared to a situation with stable climate over the next 50 y. However, model results also suggest that if global warming may have the potential of reducing the environmental levels of these chemicals, it would probably enhance their mobility and hence their potential for long range atmospheric transport.  相似文献   

14.
Levels and congener pattern of polychlorinated biphenyls (PCBs) were determined in samples of subcutaneous fat and liver from 27 polar foxes, Alopex lagopus, caught in Svalbard during the winter 1983-1984. In all the samples analysed the composition of individual PCB congeners was studied by comparison with 12 individual PCB congeners (IUPAC nos. 28, 52, 101, 118, 138, 153, 170, 180, 183, 194, 206 and 209). In addition, the PCB congeners nos. 99, 105, 114, 156 and 157 were determined in the fat samples. In both liver and fat samples the sum PCB was calculated based on the concentrations of seven selected congeners, nos. 138, 153, 170, 180, 194, 206 and 209. These congeners were the same as those used in a corresponding investigation made on arctic fox from Svalbard 10 years earlier. The present study reveals that the PCB levels in arctic fox in Svalbard are high and essentially unchanged in the period from 1973-1974 to 1983-1984. The mean sum PCB levels in fat and liver were 8.3 +/- 11 and 0.4 +/- 0.4 microg g(-1), and the extractable fat was 81.2 +/- 8.4 and 4.5 +/- 1.7% for the two tissues, respectively. In fat, sum PCB ranged from 0.5 to 41.0 microg g(-1). PCB nos. 153 and 180 accounted for approximately 65% of sum PCB. The contributions of PCB nos. 138 and 153 to the sum PCB were found to increase from 1974 to 1984. The PCB congener pattern is similar to that found in polar bears, and is dominated by a few congeners (99, 138, 153, 170, 180 and 194). No significant differences in PCB levels were found between sexes or between age groups. However, significantly higher PCB levels were found in old animals (>/= 3 years) with less than 2 cm of fat on the ramp as compared with young animals (1-2 years) with more than 2 cm of fat on the rump. Effects on vital functions from the observed levels of PCBs cannot be excluded for the most contaminated foxes.  相似文献   

15.
This paper estimates the present UK environmental loading of polychlorinated biphenyls (PCBs). Of the estimated approximately 40,000 t SigmaPCB sold in the UK since 1954, only an estimated 1% (400 t) are now present in the UK environment. Comparisons of estimated production and current environmental loadings of congeners 28, 52, 101, 138, 153 and 180 suggest that PCB persistence broadly increases with increasing chlorination. Those PCBs that are not now present in the UK environment are considered to have been destroyed--by natural or anthropogenic mechanisms, to be still in use, to reside in landfills or to have undergone atmospheric and/or pelagic transport from the UK. The dramatic fall in PCB levels in archived UK soils and vegetation between the mid-1960s and the present is evidence that the latter mechanism is the most important and that a significant proportion of PCBs released into the UK environment in the 1960s have subsequently undergone environmental transport away from the UK. The bulk (93.1%) of the estimated contemporary UK environmental burden of SigmaPCBs is associated with soils, with the rest found in seawater (3.5%) and marine sediments (2.1%). Freshwater sediments, vegetation, humans and sewage sludge combined account for 1.4% of the present burden, whilst PCB loadings in air and freshwater are insignificant. Although consideration of individual congeners does not reveal any major deviations from the relative partitioning of Sigma PCBs, the importance of sinks other than soils is enhanced for individual congeners, particularly 138 and 180. In particular, around 2% of the total UK burden of congener 180 is present in humans, implying that biodata as a whole may constitute an important sink for the higher chlorinated congeners. The contemporary flux of SigmaPCBs to the UK surface is estimated at 19 t yr(-1), compared with an estimated annual flux to the atmosphere of 44-46 t. This implies that the major sources of PCBs to the UK atmosphere have been identified and that there is currently a net loss of these compounds from the UK. These sources are: volatilisation from soils (88.1%), leaks from large capacitors (8.5%), the production of refuse-derived fuel (RDF) (2.2%), leaks from transformers (0.6%), the recovery of contaminated scrap metal (0.5%) and volatilisation from sewage sludge-amended land (0.2%). Interestingly, whilst large excesses of estimated annual fluxes to the atmosphere over deposition fluxes for individual congeners exist for congeners 28, 52 and 101, estimates of fluxes in both directions across the soil-atmosphere interface agree closely for congeners 138, 153 and 180. This suggests that lower chlorinated congeners are more susceptible to both long-range environmental transport beyond the UK and to atmospheric degradation. Retrospective analysis of dated sediment cores, vegetation and soils indicates that environmental transport from North America and continental Europe introduced PCBs into the British environment well before the onset of their commercial production in the UK in 1954. Since that time, the input of PCBs to the UK environment has essentially reflected temporal trends in UK use. After peaking in the 1960s they declined rapidly through the 1970s following restrictions on PCB use. Recent evidence, however, is that the rate of decrease has diminished and that further significant reductions in fresh environmental input will take some time to occur. Such reductions will be especially slow for humans and other biota with long life-spans. This stems partly from cross-generational transfer from parents to offspring and also because the persistence of PCBs in biota means that present body burdens will reflect past as well as current exposure.  相似文献   

16.
Eighteen teachers from a highly contaminated school and 11 teachers from a control school participated in this study. Total polychlorinated biphenyl (PCB) indoor air concentration (six indicator congeners x 5) was beyond 12000 ng/m3 in some rooms of the contaminated school. PCB 28 and PCB 52 were the prevailing congeners. Whole blood was taken from each participant by the local health authority, pooled in two groups and analysed for the six PCB indicator congeners, non-ortho PCBs and polychlorinated dibenzodioxins (PCDD)/polychlorinated dibenzofurans (PCDF). Blood analysis showed elevated mean PCB 28 and PCB 52 levels for the exposed group, however the two groups were almost identical with regard to PCB 101, 138, 153 and 180. Moreover no difference can be observed for the concentration of non-ortho PCBs and PCDD/PCDF. The data support the finding, that heavy indoor air contamination with low chlorinated PCBs causes an increase of PCB 28 and PCB 52 blood levels. However, this increment was small compared to their total PCB load.  相似文献   

17.
An assessment of PCB and PBDE contamination of surface sediments in Monastir Bay was carried out in two contrasted seasons of the year. Samples were collected from 5 sites and analyzed for the ∑7 marker PCBs (i.e. PCBs 28, 52, 101, 118, 138, 153 and 180) and ∑4 PBDE congeners (PBDEs 47, 99, 119 and 153) by GC/ECD. Concentrations of both PCBs and PBDEs showed seasonal variations. PCB concentrations were in the range of 3.1–9.3 ng g−1 and 1.1–8.1 ng g−1 in wet and dry season respectively, and sediments were considered moderately contaminated with PCBs. All PCBs analyzed were detected in surface sediments. PCB 153 and 52 congeners showed the highest relative abundance in both winter and summer. PBDE concentrations ranged from not detect to 0.1 ng g−1, with only BDE-47 congener detected in sediments and only in winter. Analysis of spatial and seasonal variations indicated that PCB distribution is governed by hydrodynamics and temporal variability of inputs. While the PCB contamination appeared to be mainly land-based, PBDEs are suspected to originate from atmospheric deposition.  相似文献   

18.
Gibson R  Wang MJ  Padgett E  Beck AJ 《Chemosphere》2005,61(9):1336-1344
When sewage sludge is added to agricultural land, organic chemicals contaminants are also added. The fate of these chemicals, particularly those shown to have oestrogenic potential, has received much research and regulatory interest in recent years. A method was developed for the analysis of 4-nonylphenols, phthalates, and PCB congeners in soils, mesophilic anaerobially digested dewatered (MADD) sewage sludge, and MADD sludge-amended soil. After Soxhlet-extraction, the 4-nonylphenols and phthalates were separated from the PCBs on an isolute cyanopropyl SPE cartridge and analysed by GC-MS directly. The PCBs were acid treated on a Bakerbond PCB-A cartridge, then passed through a gel filtration column of Biobeads SX-3 resin, before GC-MS analysis. The method was successfully validated and then used for routine analysis, where average recoveries of the surrogate standards were 83+/-17% (4-n-heptylphenol), 96+/-11% (dimethyl-tere-phthalate), 101+/-12% (dibenzyl-phthalate), and 79+/-13% (PCBs 6, 54, 104, 155, and 198).  相似文献   

19.
Soil and sediment samples from James Ross Island were analyzed for their PCB, OCP and PAH contents. Soil concentrations ranged between 0.51 and 1.82 ng g(-1) for seven indicator PCB congeners, between 0.49 and 1.34 ng g(-1) for HCH congeners, between 0.51 and 3.68 ng g(-1) for the sum of p,p'-DDT, DDE, and DDD, and between 34.9 and 171 ng g(-1) for the sum of 16 EPA PAHs. Sediment levels from 0.32 to 0.83 ng g(-1) were found for PCBs, from 0.14 to 0.76 ng g(-1) for HCHs, from 0.19 to 1.15 ng g(-1) for DDTs, and from 1.4 to 205 ng g(-1) for PAHs. A prevalence of low-mass PAHs, less chlorinated PCBs, and more volatile chemicals indicates that the long-range atmospheric transport from populated areas of Africa, South America, and Australia is the most probable contamination source for the solid matrices in James Ross Island.  相似文献   

20.
Polychlorinated biphenyls in digested UK sewage sludges   总被引:1,自引:0,他引:1  
Twelve sewage sludges from rural, urban and industrial waste water treatment works in north west England were analysed for polychlorinated biphenyls by capillary GC-ECD. The total polychlorinated biphenyl content ranged between 106 to 712 μg/kg, with a mean of 292 μg/kg. Di- and penta-chlorinated congeners made the greatest contribution to the ΣPCB concentrations at most sites. The 6 IUPAC congeners were found in the following order of abundance, 101>180>153>138>52>28. Industrial inputs would appear to influence levels of ΣPCB in the sludge.

If these sludges were ploughed into arable land at typical rates only a slight elevation in soil ΣPCB levels would result. Alternatively, if the same quantity of sludge were applied to the surface of pasture grassland, significant elevations in the potential transfer of PCBs to grazing livestock may result.  相似文献   


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