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1.
Black carbon in Slovenian alpine lacustrine sediments   总被引:11,自引:0,他引:11  
Muri G  Cermelj B  Faganeli J  Brancelj A 《Chemosphere》2002,46(8):1225-1234
Black carbon (BC) contents were measured in recent sediments in five high altitude remote alpine lakes, i.e. Lake Krisko Sup., Lake Ledvica, Lake Planina, Lake Krn and Lovrensko Lake, and the eutrophic subalpine Lake Bled in Slovenia to follow the history of atmospheric pollution of fossil fuel and local biomass burning in Alps. Organic carbon (OC), its 13C values, total nitrogen and sedimentation rates using 210Pb activity data were also measured. The highest BC contents, reaching 20 mg/gdw, were noted in remote alpine lakes while in the subalpine Lake Bled sediment the concentrations were lower reaching 5 mg/gdw. Lower BC/OC ratios, ranging between 4% and 8%, were typical for remote alpine lakes and increased to about 10% in subalpine Lake Bled. The latter clearly shows the marked importance of local direct pollution sources in comparison to remote atmospheric input which decreases in a W-E direction in parallel with decreasing amounts of precipitation. Based on 210Pb sedimentation data, the minimal BC accumulation rates in sediment cores were detected in the pre-industrialisation period. In the last decades of 20th century the BC contents decreased probably due to reduced emission of pollutants.  相似文献   

2.
Sediment cores from four Chilean lakes along the Andes Chain (Chungará, Laja, Castor and Venus) were analysed in order to investigate PCB concentrations and distributions in sediment samples. Sediment cores were analysed for PCBs using gas chromatography (GC-ECD/MS) and radioisotopically dated using 210Pb. Organic carbon content (OC) and 210Pb fluxes were also measured. Results showed that sediment PCB concentrations (ngg(-1) d.w.) at Lake Chungará (1.2 +/- 1) in northern Chile, Laja (5 +/- 4) in central, and in Lake Castor (3.5 +/- 4) in southern Chile (the eastern side of the Andes Mountain) were lower than sediments collected from Lake Venus (64 +/- 30) located in southern Chile (the western side) which contained 15-fold higher concentrations of PCBs. The percentage (%) of organic carbon was variable and showed a high range of values in the sediment fluctuating from 2% (Lake Laja) to 22% (Lake Chungará). Analysis of 210Pb fluxes, presented a decrease trend following Lake Laja>Castor>Chungará with a positive correlation with rainfall at each site. Sedimentation rates in Lake Castor (1846 gm(-2)yr(-1)) were higher than at Chungará (748 gm(-2)yr(-1)) and Lake Laja (508 gm(-2)yr(-1)). Focusing factor (FF) is used as a tool to elucidate PCB input in the aquatic ecosystem. FF were lower (<1) for the shallower lakes (Lakes Chungará and Castor). This study provides background levels of PCBs at remote lakes in Chile. Differences in geographical characteristics (orographic effect) might play an important role in the arrival of PCBs, particularly into the southern lakes. PCB fluxes indicated deposition of PCBs in recent sediments is higher than in previous years with peaks of PCB between 1991 and 1998. The continuing increase of PCB inputs in remote Chilean lakes, could be associated with long range atmospheric transport (LRAT).  相似文献   

3.
Distributions of total organic carbon (TOC), black carbon (BC), and polycyclic aromatic hydrocarbons (PAH) were investigated in different particle size fractions for four Norwegian harbor sediments. The total PAH (16-EPA) concentrations ranged from 2 to 113 mg/kg dry weight with the greatest fraction of PAH mass in the sand fraction for three of the four sediments. TOC contents ranged from 0.84% to 14.2% and BC contents from 0.085% to 1.7%. This corresponds to organic carbon (OC = TOC - BC) contents in the range of 0.81-14% and BC:TOC ratios of 1.3-18.1%. PAH isomer ratios suggested that the PAH in all four sediments were of pyrogenic origin. Furthermore, stronger correlations between PAH versus BC (r2 = 0.85) than versus OC (r2 = 0.15) were found. For all size fractions and bulk sediments, the PAH-to-BC ratios for the total PAHs were on average 6+/-3 mg PAH/g BC. These results suggest that PAH distributions were dominated by the presence of BC, rather than OC. As sorption to BC is much stronger than sorption to OC, this may result in significantly lower dissolved concentrations of PAH than expected on the basis of organic carbon partitioning alone.  相似文献   

4.
Snow cores were collected in the catchment area of five remote mountain lakes in Europe. They were analysed for polycyclic aromatic hydrocarbons (PAH), polychlorinated biphenyls (PCB), and organochlorine pesticides, namely DDTs, hexachlorobenzene (HCB) and hexachlorocyclohexanes (HCH). PAH are found in higher amounts in the Tatra and Caledonian mountains, PCB are higher in the Alps and HCH are highest in the Alps and Pyrenees. The qualitative PAH distributions are dominated by low molecular weight compounds, phenanthrene being the most abundant PAH in all but in one site. These compounds also occur predominantly in the gas phase in the atmosphere. Their high abundance in the snowpack witness the occurrence of effective transfer mechanisms from gas to snow flakes. In Starolesnianske (Tatra mountains), a higher contribution of high molecular weight compounds is found. This site exhibits the highest snow PAH and suspended particulate levels. Transformation of the concentration values of these compounds into annual deposition rates and correction for catchment/lake area indicates that in Scandinavia and the Alps a large proportion of PAH incorporation is mediated by snowfallout whereas in the Tatra mountains snow deposition only accounts for a small fraction of the compounds stored in the lake sediments. Among organochlorine compounds, only PCB and HCH have been found above method detection limit in most of the samples. The PCB congener distributions changes significantly between sites, although a predominance of the less chlorinated congeners have generally been observed.  相似文献   

5.
Surface sediments from remote lakes and coastal areas from Ny-Ålesund, Svalbard, Norwegian Arctic were analyzed for polycyclic aromatic hydrocarbons (PAHs), polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs). Relatively high levels of PAHs were encountered from several lakes from Ny-Ålesund, which were within the range of levels reported for European high mountain lakes and some urban/industrialized areas in the world, pointing to the role of remote Arctic lakes as potential reservoir of semi-volatile organic compounds. Specific patterns of PBDEs were observed, showing higher concentrations of lower brominated compounds such as BDE-7, 17 and 28. Estimated surface sediment fluxes of PAHs in Ny-Ålesund remote lakes were similar to those observed for some European high mountain lakes. The current PAH levels in sediments from three lakes exceeded Canadian sediment quality guidelines, suggesting the presence of possible risks for aquatic organisms and the need for further studies.  相似文献   

6.
European alpine lake systems are used as indicators of air quality over the continent. Preliminary data showed high polycyclic aromatic hydrocarbons (PAH) loads in the High Tatras (Eastern Europe) in comparison to other mountain regions. Here, insight on the spatial distribution of PAH is provided from analysis of top-core sediments of 27 alpine lakes distributed along the High Tatras.Top-core sediment concentrations were higher than those in deep-cores, and they were higher than those observed in other European high mountain regions. The PAH profiles were uniform and comparable to those observed in aerosols and snow, indicating that atmospheric deposition was the predominant PAH input pathway to the lakes. Good agreement between estimated atmospheric deposition and sedimentation fluxes was observed. However, in several lakes in the western range higher sediment fluxes may correspond to higher PAH depositions levels. The higher concentrations may also reflect inputs from potential emission source areas.  相似文献   

7.
Polycyclic aromatic hydrocarbons (PAH) were analysed in 23 soil samples (0–10 cm layer) from the Swiss soil monitoring network (NABO) together with total organic carbon (TOC) and black carbon (BC) concentration, as well as some PAH source diagnostic ratios and molecular markers. The concentrations of the sum of 16 EPA priority PAHs ranged from 50 to 619 μg/kg dw. Concentrations increased from arable, permanent and pasture grassland, forest, to urban soils and were 21–89% lower than median numbers reported in the literature for similar Swiss and European soils. NABO soils contained BC in concentrations from 0.4 to 1.8 mg/g dw, except for two sites with markedly higher levels. These numbers corresponded to 1–6% of TOC and were comparable to the limited published BC data in soil and sediments obtained with comparable analytical methods. The various PAH ratios and molecular markers pointed to a domination of pyrogenically formed PAHs in Swiss soils. In concert, the gathered data suggest the following major findings: (1) gas phase PAHs (naphthalene to fluorene) were long-range transported, cold-condensated at higher altitudes, and approaching equilibrium with soil organic matter (OM); (2) (partially) particle-bound PAHs (phenanthrene to benzo[ghi]perylene) were mostly deposited regionally in urban areas, and not equilibrated with soil OM; (3) Diesel combustion appeared to be a major emission source of PAH and BC in urban areas; and (4) wood combustion might have contributed significantly to PAH burdens in some soils of remote/alpine (forest) sites.  相似文献   

8.
Organic pollutants (e.g. polyaromatic hydrocarbons (PAH)) strongly sorb to carbonaceous sorbents such as black carbon and activated carbon (BC and AC, respectively). For a creosote-contaminated soil (Sigma15PAH 5500 mg kg(dry weight(dw))(-1)) and an urban soil with moderate PAH content (Sigma15PAH 38 mg kg(dw)(-1)), total organic carbon-water distribution coefficients (K(TOC)) were up to a factor of 100 above values for amorphous (humic) organic carbon obtained by a frequently used Linear-Free-Energy Relationship. This increase could be explained by inclusion of BC (urban soil) or oil (creosote-contaminated soil) into the sorption model. AC is a manufactured sorbent for organic pollutants with similar strong sorption properties as the combustion by-product BC. AC has the potential to be used for in situ remediation of contaminated soils and sediments. The addition of small amounts of powdered AC (2%) to the moderately contaminated urban soil reduced the freely dissolved aqueous concentration of native PAH in soil/water suspensions up to 99%. For granulated AC amended to the urban soil, the reduction in freely dissolved concentrations was not as strong (median 64%), especially for the heavier PAH. This is probably due to blockage of the pore system of granulated AC resulting in AC deactivation by soil components. For powdered and granulated AC amended to the heavily contaminated creosote soil, median reductions were 63% and 4%, respectively, probably due to saturation of AC sorption sites by the high PAH concentrations and/or blockage of sorption sites and pores by oil.  相似文献   

9.
Relations between urbanization and particle-associated contaminants in New England were evaluated using a combination of samples from sediment cores, streambed sediments, and suspended stream sediments. Concentrations of PAHs, PCBs, DDT, and seven trace metals (Cd, Cr, Cu, Hg, Ni, Pb, Zn) were correlated strongly with urbanization, with the strongest relations to percentage commercial, industrial, and transportation (CIT) land use. Average PAH and metal concentrations in the most urbanized watersheds were approximately 30 and 6 times the reference concentrations, respectively, in remote, undeveloped watersheds. One-quarter to one-half of sampling sites had concentrations of PAHs, Cu, Pb, or Zn above the probable effects concentration, a set of sediment quality guidelines for adverse effects to aquatic biota, and sediments were predicted to be toxic, on average, when CIT land use exceeded about 10%. Trends in metals in cores from urban watersheds were dominantly downward, whereas trends in PAHs in a suburban watershed were upward. A regional atmospheric-fallout gradient was indicated by as much as order-of-magnitude-greater concentrations and accumulation rates of contaminants in cores from an undeveloped reference lake in Boston compared to those from remote reference watersheds. Contaminant accumulation rates in the lakes with urbanization in their watersheds, however, were 1-3 orders of magnitude greater than those of reference lakes, which indicate the dominance of local sources and fluvial transport of contaminants to urban lakes. These analyses demonstrate the magnitude of urban contamination of aquatic systems and air sheds, and suggest that, despite reductions in contaminant emissions in urban settings, streams and lakes will decline in quality as urbanization of their watersheds takes place.  相似文献   

10.
Sediment cores taken from the deep basin of Loch Coire nan Arr in north-west Scotland were dated using 210Pb calibrated spheroidal carbonaceous particle (SCP) profiles and analysed for trace metals, polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs). These data show that the site is one of the least contaminated by atmospheric pollution in the UK. Peak concentrations of PAHs were found to be equivalent to background values at sites in the English Lake District. The date of concentration maxima for SCP, PCB and some metals were in agreement with previously published polychlorinated dibenzo-p-dioxin/polychlorinated dibenzofuran (PCDD/F) data suggesting long-range industrial sources. The date of individual PAH concentration maxima were earlier, but concomitant with each other, possibly suggesting the influence of a local source. Comparison with remote European mountain lakes shows Loch Coire nan Arr to be one of the least contaminated sites in Europe with respect to PCBs, but more contaminated with respect to PAHs.  相似文献   

11.
The concentrations of total polycyclic aromatic hydrocarbons (sigmaPAHs) and 15 individual PAH compounds in 20 surface sediments collected from four mangrove swamps in Hong Kong were analysed. sigmaPAH concentrations ranged from 356 to 11,098 ng g(-1) dry weight with mean and median values of 1992 and 1,142 ng g(-1), respectively. These values were significantly higher than those of marine bottom sediments of Hong Kong harbours, suggesting that more PAHs were accumulated in mangrove surface sediments. The concentrations of sigmaPAHs as well as individual PAH compound varied significantly among mangrove swamps. The swamps heavily polluted by livestock and industrial sewage, such as Ho Chung and Mai Po, had much higher concentrations of total PAHs and individual PAH than the other swamps. The PAH profiles were similar among four mangrove swamps, and were dominated by naphthalene (two-ring PAH), fluorene and phenanthrene (three-ring PAH). The mangrove sediments had higher percentages of low-molecular-weight PAHs. These indicated that PAHs in mangrove sediments might originate from oil or sewage contamination (petrogenic input). Ratio values of specific PAH compounds such as phenanthrene/anthracene and fluoranthene/ pyrene, were calculated to evaluate the possible source of PAH contamination in mangrove sediments. These ratios varied among samples, suggesting that mangrove sediments might have a mixed pattern of pyrolytic and petrogenic inputs of PAHs. Sediments collected from Ho Chung mangrove swamp appeared to be more dominated by pyrolytic input while those from Tolo showed strong petrogenic contamination.  相似文献   

12.
The levels and distribution of polynuclear aromatic hydrocarbons (PAHs) were determined in soil samples from background locations in the UK and Norway, to investigate their spatial distribution and the controlling environmental factors. Concentrations ranged between 42 and 11200 microg kg(-1) (geometric mean 640 microg kg(-1)) and 8.6 and 1050 microg kg(-1) (150 microg kg(-1)) dry weight in the UK and Norwegian soil, respectively. Proximity to sources and locations susceptible to high atmospheric depositional inputs resulted in higher concentrations. Statistically significant relationships were observed between PAH and total organic carbon (TOC) in the Norwegian samples. High molecular weight PAHs correlated with black carbon (BC) in UK-woodland soil. These observations support the hypothesis that TOC plays an important role in the retention of PAHs in soil and that PAHs are often combined with BC during combustion emissions. PAHs with 4 and more rings comprised approximately 90% of total PAHs in the UK soil, but only 50% in the Norwegian soil. The mixture of PAHs implied that fractionation occurred during long-range atmospheric transport and deposition. The lighter PAHs with lower K(ow) values more readily reached the most remote sites. The heavier PAHs with higher K(ow) values remained in closer proximity to sources.  相似文献   

13.
The contents of nonhydrolyzable organic matter (NHC) and black carbon (BC) were measured in soils and sediments from the Pearl River Delta, South China. Polycyclic aromatic hydrocarbons (PAHs) were extracted respectively by Soxhlet and an accelerated solvent extraction device (ASE) using different solvents. In addition, sequential aqueous leaching at different temperatures was carried out. The PAH content extracted with the sequential three solvent ASE is two times higher than that using the Soxhlet extraction method. The relationship of the PAH content with the NHC content is very significant. The PAH concentrations measured at various temperature steps fit well to the Van't Hoff equation and the enthalpy was estimated. The investigation indicates that condensed organic matter such as kerogen carbon, aged organic matter, and BC is relevant for the extraction and distribution of native PAHs in the investigated field soils and sediments.  相似文献   

14.
Mercury contamination in Canada's Bay of Fundy is a priority concern because of elevated levels observed in fish, birds and wildlife. Salt marshes constitute an important part of the Bay's coastline and are potential stores of mercury for the region. We measured the amount of mercury accumulated over a 5-yr period from 1997 to 2002 in surface sediments of seven salt marshes along the New Brunswick coast of the Bay. The seven study sites extended from outer to inner Bay, spanning a gradient in tidal range (6-12 m) and sediment characteristics such as %LOI (4-29%) and sediment deposition rate (0.27-1.76 cm yr(-1)). In each study site, mercury was measured in low and high marsh areas. Sediment mercury concentrations ranged from 7 to 79 ng g(-1) and loading rates ranged from 0.1 to 1.1 mg m(-2). Total estimated 5-yr storage of mercury in salt marsh sediments of the Bay is 854+/-465 kg. We also compared sediment mercury loading to atmospheric inputs measured at a deposition monitoring station operating in New Brunswick from 1997 to 2002 and found that direct atmospheric deposition appears to be a minor input of mercury to these sediments. We are unaware of documentation of mercury loading in salt marshes on a bay-wide scale and over a constrained (5-yr) time period elsewhere.  相似文献   

15.
We have examined how some major catchment disturbances may affect the aquatic greenhouse gas fluxes in the boreal zone, using gas flux data from studies made in 1994-1999 in the pelagic regions of seven lakes and two reservoirs in Finland. The highest pelagic seasonal average methane (CH(4)) emissions were up to 12 mmol x m(-2) x d(-1) from eutrophied lakes with agricultural catchments. Nutrient loading increases autochthonous primary production in lakes, promoting oxygen consumption and anaerobic decomposition in the sediments and this can lead to increased CH(4) release from lakes to the atmosphere. The carbon dioxide (CO(2)) fluxes were higher from reservoirs and lakes whose catchment areas were rich in peatlands or managed forests, and from eutrophied lakes in comparison to oligotrophic and mesotrophic sites. However, all these sites were net sources of CO(2) to the atmosphere. The pelagic CH(4) emissions were generally lower than those from the littoral zone. The fluxes of nitrous oxide (N(2)O) were negligible in the pelagic regions, apparently due to low nitrate inputs and/or low nitrification activity. However, the littoral zone, acting as a buffer for leached nitrogen, did release N(2)O. Anthropogenic disturbances of boreal lakes, such as increasing eutrophication, can change the aquatic greenhouse gas balance, but also the gas exchange in the littoral zone should be included in any assessment of the overall effect. It seems that autochthonous and allochthonous carbon sources, which contribute to the CH(4) and CO(2) production in lakes, also have importance in the greenhouse gas emissions from reservoirs.  相似文献   

16.
Black carbon (BC; soot and charcoal) can be an extremely strong sorbent for organic compounds. In a previous study, sorption of d(10)-phenanthrene (d(10)-PHE) to BC in an unmodified contaminated sediment was found to be nine times less than that for BC isolated from this sediment. To find out the mechanism of this sorption attenuation (competition for BC sites between d(10)-PHE and native PAHs or blocking of BC sites by natural organic matter), we determined the effect on d(10)-PHE-BC sorption isotherms of additions of either PAHs or precipitated humic acid. Addition of humic acid did not significantly decrease BC sorption, whereas PAH additions (equal to the native PAH content in the original sediment) did, by about one order of magnitude. Therefore, competition between d(10)-PHE and the native PAHs could explain the whole attenuation of sorption to BC in unmodified sediments.  相似文献   

17.
《Environmental Forensics》2013,14(4):287-300
Polycyclic aromatic hydrocarbons (PAH) are ubiquitous constituents in urban sedimentary environments. The accurate characterization of their source(s) in sediments influences decisions regarding the liability for clean-up and remedial options. In this study, an extensive PAH dataset that included 50 non-alkylated (parent) and alkylated PAH groups and isomers was acquired using a modified EPA Method 8270 for the study of 5 cm intervals from 10 sediment cores (28-78 cm) obtained from the Eagle Harbor Superfund Site on Bainbridge Island, Washington. Conventional hydrocarbon "fingerprinting" and the PAH profiles in the Pb 210 age-dated cores revealed three primary PAH sources to the sediments over the past 220 years, namely (1) naturally occurring background; (2) urban runoff, and (3) creosote, the latter resulting from prior operations at the former Wyckoff wood-processing facility located on the Harbor. Naturally occurring background PAH in the pre-industrial (<1900) sediments were dominated by perylene, 1,7-dimethylphenan-threne (derived from the oxidation of abietic acid resins), and pyrogenic PAH most likely derived from historic forest fires. The concentration of PAH total in these pre-industrial sediments was consistently less than 1 mg/kg (dry). Urban runoff in the post-industrial (>1930) sediments was dominated by low but consistent concentrations (10-20 mg/kg dry) of pyrogenic PAM derived primarily from the combustion of fossil fuel(s). The creosote-impacted sediments in the post-industrialized sediments contained high concentrations (1000-140,000 mg/kg dry) of pyrogenic PAH associated with distilled, coal-derived liquids.  相似文献   

18.
The role of resuspension duration on release of 16 PAHs was measured experimentally using a particle entrainment simulator (PES). Three sediment cores were resuspended for 12h at 0.2 and 0.5N m(-2). PAHs in water column and total suspended solids (TSS) were monitored at intervals. After 0.25h of resuspension, PAH release was on average 42% of their concentrations after 12h of resuspension, indicating fast release of PAHs from sediments in an initial short time. Moreover, PAHs released faster at 0.5N m(-2) than at 0.2N m(-2); low molecular weight PAHs (2-3-ring) released faster than median molecular weight (4-ring) PAHs. PAH concentrations in TSS showed generally increase with time and differences in magnitudes based on sediment type and energy. Overall, the composition of sediments is the major factor in determining the amount of released PAHs, more so than the level of resuspension energy applied.  相似文献   

19.
Ek AS  Löfgren S  Bergholm J  Qvarfort U 《Ambio》2001,30(2):96-103
Copper production in Falun, central Sweden, has emitted sulfur dioxide (SO2) and metals to the air during at least 1000 years. Emissions peaked in the 17th century when Falun produced 2/3 of the world's copper supply. This area offers unique opportunities to study long-term effects of acid deposition and metal pollution, including recovery following the three centuries of decreasing SO2 and metal deposition. Here we present a 1000-yr perspective on local emissions of SO2, estimated air concentrations and dry deposition of SO2, as well as results on acidification and metal pollution of soils and lakes. Despite a long period when deposition of SO2 exceeded the critical load, soil acidification is limited to the most heavily polluted area 12 km NW and SE from the mine. According to diatom analyses of take sediments, only 8 of 14 lakes have become acidified (0.4-0.8 pH units). None of these lakes show recovery from acidification, probably due to large amounts of sulfate still accumulated in the soils and changes in land use.  相似文献   

20.
The Lot-Garonne fluvial system is known for its historic heavy metal pollution resulting from mining and smelting activities since the late 19th century. Here, we report 137Cs activities and heavy metal (Cd, Zn, Cu, Pb and V) concentration-depth profiles from sediment cores retrieved in 2001 from three reservoirs in the Lot River. High mean sedimentation rates of 2.4-2.8 cm a(-1) are indicated by 137Cs dating. The reservoir sediments have recorded the heavy metal deposition and thus allow establishing a connection between the temporal evolution of the heavy metal pollution and historical changes in smelting and waste-treatment proceedings. Based on heavy metal concentrations in sediments upstream of the anthropogenic inputs and bottom-sediments of the furthest downstream core (interpreted as old soil or riverbed), concentrations of approximately 17, approximately 82, approximately 0.33 and approximately 28 mg kg(-1) for Cu, Zn, Cd and Pb, respectively, are proposed as natural background values for the Lot fluvial system. The geoaccumulation index (Igeo [Müller, G., 1979. Schwermetalle in den Sedimenten des Rheins-Ver?nderungen seit. Umschav 79, 133-149.]) revealed that the Lot River sediments must be considered as "severely polluted" in Cd and Zn. Moreover, despite remediation efforts undertaken in the former smelting site, the Lot River is still "severely" (Igeo approximately 4) and "moderately to severely" (Igeo>2) impacted by Cd and Zn inputs, respectively.  相似文献   

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