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1.
Black carbon (BC) and total organic carbon (TOC) contents of UK and Norwegian background soils were determined and their relationships with persistent organic pollutants (HCB, PAHs, PCBs, co-planar PCBs, PBDEs and PCDD/Fs) investigated by correlation and regression analyses, to assess their roles in influencing compound partitioning/retention in soils. The 52 soils used were high in TOC (range 54-460 mg/g (mean 256)), while BC only constituted 0.24-1.8% (0.88%) of the TOC. TOC was strongly correlated (p < 0.001) with HCB, PCBs, co-PCBs and PBDEs, but less so with PCDD/Fs (p < 0.05) and PAHs. TOC explained variability in soil content, as follows: HCB, 80%; PCBs, 44%; co-PCBs, 40%; PBDEs, 27%. BC also gave statistically significant correlations with PBDEs (p < 0.001), co-PCBs (p < 0.01) and PCBs, HCB, PCDD/F (p < 0.05); TOC and BC were correlated with each other (p < 0.01). Inferences are made about possible combustion-derived sources, atmospheric transport and air-surface exchange processes for these compounds.  相似文献   

2.
Chen L  Ran Y  Xing B  Mai B  He J  Wei X  Fu J  Sheng G 《Chemosphere》2005,60(7):879-890
We investigated contents, distribution and possible sources of PAHs and organochlorine pesticides (Ops) in 43 surface and subsurface soils around the urban Guangzhou where variable kinds of vegetables are grown. The results indicate that the contents of PAHs (16 US EPA priority PAHs) range from 42 to 3077 microg/kg and the pollution extent is classified as a moderate level in comparison with other investigations and soil quality standards. The ratios of methylphenanthrenes to phenanthrene(MP/P), anthracene to anthracene plus phenanthrene (An/178), benz[a]anthracene to benz[a]anthracene plus chrysene (BaA/228), indeno[1,2,3-cd]pyrene to indeno[1,2,3-cd]pyrene plus benzo[ghi]perylene (In/In+BP) suggest that the sources of PAHs in the soil samples are mixed with a dominant contribution from petroleum and combustion of fossil fuel. The correlation analysis shows that the PAHs contents are significantly related to total organic carbon contents (TOC) (R2=0.75) and black carbon contents (BC) (R2=0.62) in the soil samples. Dichlorodiphenyltrichloroethane and metabolites (DDTs) and hexachlorocyclohexanes and metabolites (HCHs) account largely for the contaminants of OPs. The concentrations of DDTs range from 3.58 to 831 microg/kg and the ratios for DDT/(DDD+DDE) are higher than 2 in some soil samples, suggesting that DDT contamination still exists and may be caused by its persistence in soils and/or impurity in the pesticide dicofol. The concentrations of HCHs are 0.19-42.3 microg/kg.  相似文献   

3.
We determined 20 polycyclic aromatic hydrocarbons (PAHs) and 12 polychlorinated biphenyls (PCBs) in Oi, Oe, and Oa horizons and at 0-5 and 15-20 cm mineral soil depth of 16 Norway spruce (Picea abies) stands in north Bavaria. The sum of PAH concentrations increased along the line Oi (mean+/-SD: 841+/-330 microg kg(-1))相似文献   

4.
The influence of black carbon (BC) on the sorption of 17 native polychlorinated-p-dibenzodioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) was studied in five soil samples from a sawmill site where wood used to be impregnated with chlorophenol preservatives. The presence of BC caused measured total organic carbon (TOC)-water distribution ratios (K(TOC)) to be a median factor of 51 (interquartile range 18-68, n=85) higher than modeled amorphous organic carbon (AOC)-water distribution ratios (K(AOC)). K(TOC) was a factor of 73+/-27 above K(AOC) for PCDFs (n=10) and a factor of 20+/-13 (n=7) for PCDDs. The reason for this difference is probably that attaining a planar configuration after sorption to BC is less thermodynamically favorable for PCDDs than for PCDFs. BC-water distribution ratios were calculated from K(TOC), K(AOC) and BC contents, and ranged from 10(9.9) (2,3,7,8-Tetra-CDD) to 10(11.5) l kg(-1) (Octa-CDF). More than 90% of the PCDD/Fs in the soil was calculated to be BC-sorbed. Dissolved organic carbon (DOC)-water distribution ratios were measured to be in the same order of magnitude as K(AOC). This study shows that strong sorption to BC should be included when assessing ecotoxicological risk or modeling transport to groundwater of PCDD/Fs in soil.  相似文献   

5.
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   

6.
Polycyclic aromatic hydrocarbons (PAHs) were quantified in 30 soil profiles from the Yangtze River Delta Region, in east China. Relative concentrations of PAH compounds with different benzene rings and ratios of fluoranthene to fluoranthene plus pyrene and benz(a)anthracene to benz(a)anthracene plus chrysene were used to identify the possible sources of soil PAHs. Total concentrations of 15 PAHs in topsoils ranged from 8.6 to 3881 microg kg(-1) with an average of 397 microg kg(-1). Half of the soil samples were considered to be contaminated with PAHs (>200 microg kg(-1)) and two sampling sites were heavily polluted by PAHs with concentrations >1000 microg kg(-1). Phenanthrene was found in soils below a depth of 100 cm in half of the sampling sites, but the detectable ratio of benzo(a)pyrene decreased sharply from 100% in topsoil to 0 in the 4th horizon.  相似文献   

7.
We determined the concentrations of 35 PCNs, 12 PCBs, and 20 PAHs in 49 urban topsoils under different land use (house garden, roadside grassland, alluvial grassland, park areas, industrial sites, agricultural sites) and in nine rural topsoils. The sums of concentrations of 35 PCNs (sigma35 PCNs) were <0.1-15.4 microg kg(-1) in urban soils and <0.1 to 0.82 microg kg(-1) in rural soils. The PCN, PCB, and PAH concentrations were highest at industrial sites and in house gardens. While rural soils receive PCNs, PCBs, and PAHs by common atmospheric deposition, there are site-specific sources of PCNs, PCBs, and PAHs for urban soils such as deposition of contaminated technogenic materials. The PCN, PCB, and PAH concentrations decreased from the central urban to the rural area. In the same order the contribution of lower chlorinated PCNs and PCBs increased because they are more volatile and subject to increased atmospheric transport. The PCNs 52+60, and 73 were more abundant in soil samples than in Halowax mixtures, indicating that combustion contributed to the PCN contamination of the soils.  相似文献   

8.
Liu S  Xia X  Zhai Y  Wang R  Liu T  Zhang S 《Chemosphere》2011,82(2):223-228
The concentrations of black carbon (BC), total organic carbon (TOC) and polycyclic aromatic hydrocarbons (PAHs) have been determined in soils from urban and rural areas of Beijing. The rural area can be divided into plain and mountainous areas which are close to and relatively far from the urban area, respectively. Concentration of BC (5.83 ± 3.05 mg g−1) and BC/TOC concentration ratio (0.37 ± 0.15) in Beijing’s urban soil are high compared with that in world background soils and rural soils of Beijing, suggesting the urban environment to be an essential source and sink of BC. Concentration of BC in the urban area decreases from the inner city to exterior areas, which correlates with the urbanization history of Beijing and infers accumulation of BC in old urban soils. Black carbon in Beijing soils mainly comes from fossil fuel combustion, especially traffic emission. Median PAH concentration in the urban area (502 ng g−1) is one order of magnitude higher than that in the rural plain (148 ng g−1) and mountainous area (146 ng g−1) where PAHs are supposed to mainly come from atmospheric deposition from the urban area. Concentrations of BC correlate significantly with those of PAHs (p < 0.01, except naphthalene) in the urban area and with those of heavier 4-, 5- and 6- ring PAHs (p < 0.01) in the adjacent rural plain area, while there is no significant correlation with any PAH in the farther rural mountainous area.  相似文献   

9.
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   

10.
Krauss M  Wilcke W 《Chemosphere》2005,59(10):1507-1515
The sorption strength of persistent organic pollutants in soils may vary among different soil organic matter (SOM) pools. We hypothesized that polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) were unevenly distributed and had different soil organic carbon (SOC)-water partition coefficients (K(OC)) among soil density fractions. We determined the concentrations and K(OC) values of 20 PAHs and 12 PCBs in bulk samples and three density fractions (light, <2.0, medium, 2.0-2.4, and heavy, >2.4 g cm(-3)) of 11 urban topsoils (0-5 cm) from Bayreuth, Germany. The K(OC) values were determined using sequential extraction with methanol-water mixtures (35% and 65% methanol) at 60 degrees C. The sum of 20 PAH concentrations in bulk soil ranged 0.4-186 mg kg(-1), and that of 12 PCB concentrations 1.2-158 microg kg(-1). The concentrations of all PAHs and PCBs decreased in the order light>medium>heavy fraction. When normalized to the SOC concentrations, PAH concentrations were significantly higher in the heavy than in the other density fractions. The K(OC) values of the PAHs in density fractions were 3-20 times higher than those of the PCBs with similar octanol-water partition coefficients (K(OW)). The K(OC) values of individual PAHs and PCBs varied up to a factor of 1000 among the studied soils and density fractions. The K(OC) values of 5- and 6-ring PAHs tended to be highest in the heavy fraction, coinciding with their enrichment in this fraction. For the other PAHs and all PCBs, the K(OC) values did not differ among the density fractions. Thus, there is no relationship between sorption strength and distribution among density fractions, indicating that density fractionation is not a suitable tool to distinguish among differently reactive PAH and PCB pools in soils.  相似文献   

11.
Marine culture is thriving in China and represents a major component of the regional economy in coastal zones, yet the environmental quality of many of those areas has never been studied. This paper attempts to investigate the quality status of Daya Bay, a key aquaculture area in China. The levels of 16 polycyclic aromatic hydrocarbons (PAHs) were determined in water and sediment samples of the bay. The total concentrations of 16 PAHs varied from 4228 to 29325 ng l(-1) in water, and from 115 to 1134 ng g(-1) dry weight in sediments. In comparison to many other marine systems studied, the PAH levels in Daya Bay waters were relatively high, and at six sites they were sufficiently high (> 10 microg l (-1)) to cause acute toxicity. The PAH composition pattern in sediments suggest dominance by medium to high molecular weight compounds, and the ratio of certain related PAHs indicate important pyrolytic and petrogenic sources. Further analysis showed that the distribution coefficient (KD) increased with the particular organic carbon content of sediments, consistent with the PAH partition theory. The organic carbon normalised distribution coefficient (K(oc)) also increased with the compounds' octanol/water partition coefficient (K(ow)), confirming the potential applicability of the linear free energy relationships in the modelling and prediction of PAH behaviour in marine environments.  相似文献   

12.
Persistent organic pollutants (PAHs and PCBs) in soil samples from seven sites across the Seine basin were analysed. Samples were taken from industrialized, urban, suburban and remote sites. Results showed spatial differences, in terms of concentrations and congener profiles. PAH (Sigma14 PAHs) and PCB (Sigma 7 PCBs) concentrations ranged from 450 to 5650 microg kg(-1) and 0.09 to 150 microg kg(-1), respectively. A clear gradient from industrial to remote sites was highlighted, with a ratio of up to one order of magnitude for PAHs and two orders of magnitude for PCBs. Fluoranthene and pyrene were predominant, while the carcinogenic PAHs represented 15-46% of the total PAH content. Using hierarchical cluster analysis, soil samples profiles were compared and the influence of site location and potential sources were identified: automobile traffic, domestic heating, and industrial emissions were the prevalent PAHs sources in the Seine basin. PCB profiles suggested different transport patterns among congeners. For remote sites, the congener fingerprint showed a relatively higher proportion of the most volatile congeners, which were attributed to increased atmospheric residence times. Thus, PAH and PCB distributions in soils provided information on sources and evidence for short-range transport, and profiles of compounds reflected differences between regional and local emissions. This study demonstrates that soil sampling can be used to investigate spatial differences in atmospheric inputs of persistent organic pollutants based on differences in the mixtures of compounds, reflecting differences in regional and local atmospheric emissions.  相似文献   

13.
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   

14.
Martins M  Ferreira AM  Vale C 《Chemosphere》2008,71(8):1599-1606
Depth concentration profiles of PAHs, organic carbon and dissolved oxygen in non-colonised sediments and sediments colonised by Sarcocornia fruticosa from Mitrena salt marsh (Sado, Portugal) were determined in November 2004 and April 2005. Belowground biomass and PAH levels in below and aboveground material were also determined. In both periods, colonised sediments were oxygenated until 15-cm, rich in organic carbon (max 4.4%) and presented much higher PAH concentrations (max. 7.1 microg g(-1)) than non-colonised sediments (max. 0.55 microg g(-1)). Rooting sediments contained the highest PAH concentrations. The five- and six-ring compounds accounted to 50-75% of the total PAHs in colonised sediments, while only to 30% in non-colonised sediments. The elevated concentrations of PAHs in colonised sediments may be attributed to the transfer of dissolved PAH compounds towards the roots as plant uptake water and subsequent sequestration onto organically rich particles. A phase-partitioning mechanism probably explains the higher retention of the heavier PAHs. In addition oxygenated conditions of the rooting sediments favour the degradation of the lighter PAHs and explain the elevated proportion of the heavier compounds. Below and aboveground materials presented lower PAH concentrations (0.18-0.38 microg g(-1)) than colonised sediments. Only 3- and 4-PAHs were quantified in aboveground material, reflecting either preferential translocation of lighter compounds from roots or atmospheric deposition.  相似文献   

15.
The concentrations, profiles, sources and spatial distribution of polycyclic aromatic hydrocarbons (PAHs) were determined in 40 surface soil samples collected from Beijing, Tianjin and surrounding areas, North China in 2007, and all sampling sites were far from industrial areas, roadsides and other pollution sources, and across a range of soil types in remote, rural villages and urban areas. The total concentrations of 16 PAHs ranged from 31.6 to 1475.0 ng/g, with an arithmetic average of 336.4 ng/g. The highest PAH concentrations were measured in urban soils, followed by rural village soils and soils from remote locations. The remote-rural village-urban PAH concentration gradient was related to population density, gross domestic product (GDP), long-range atmospheric transport and different types of land use. In addition, the PAH concentration was well correlated with the total organic carbon (TOC) concentration of the soil. The PAH profile suggested that coal combustion and biomass burning were primary PAH sources.  相似文献   

16.
To distinguish between pyrogenic and biological sources of PAHs in a tropical rain forest near Manaus, Brazil, we determined the concentrations of 21 PAHs in leaves, bark, twigs, and stem wood of forest trees, dead wood, mineral topsoil, litter layer, air, and Nasutitermes termite nest compartments. Naphthalene (NAPH) was the most abundant PAH with concentrations of 35 ng m(-3) in air (>85% of the sum of 21PAHs concentration), up to 1000 microg kg(-1) in plants (>90%), 477 microg kg(-1) in litter (>90%), 32 microg kg(-1) in topsoil (>90%), and 160 microg kg(-1) (>55%) in termite nests. In plants, the concentrations of PAHs in general decreased in the order leaves > bark > twigs > stem wood. The concentrations of most low-molecular weight PAHs in leaves and bark were near equilibrium with air, but those of NAPH were up to 50 times higher. Thus, the atmosphere seemed to be the major source of all PAHs in plants except for NAPH. Additionally, phenanthrene (PHEN) had elevated concentrations in bark and twigs of Vismia cayennensis trees (12-60 microg kg(-1)), which might have produced PHEN. In the mineral soil, perylene (PERY) was more abundant than in the litter layer, probably because of in situ biological production. Nasutitermes nests had the highest concentrations of most PAHs in exterior compartments (on average 8 and 15 microg kg(-1) compared to <3 microg kg(-1) in interior parts) and high PERY concentrations in all compartments (12-86 microg kg(-1)), indicating an in situ production of PERY in the nests. Our results demonstrate that the deposition of pyrolytic PAHs from the atmosphere controls the concentrations of most PAHs. However, the occurrence of NAPH, PHEN, and PERY in plants, termite nests, and soils at elevated concentrations supports the assumption of their biological origin.  相似文献   

17.
Surface soil (0-20 cm) samples from nine representative vegetable fields located in Guangzhou, Shenzhen, Zengcheng and Huadu within the Pearl River Delta, South China were collected and analyzed for 16 USEPA priority polycyclic aromatic hydrocarbons (PAHs) using gas chromatography coupled to mass spectrometry (GC-MS). Total concentrations of 16 PAHs (Sigma(PAHs)) ranged from 160 to 3700 microg kg(-1). Large variations were observed also between concentrations of individual PAHs from different vegetable fields and within the site as well. Acenapthylene, benzo[b]fluoranthene, fluoranthene, benzo[a]pyrene and benzo[k]fluoranthene were consistently the most prevalent individual PAHs. The values of PAH isomer ratios [anthracene/(anthracene+phenanthrene) and fluoranthene/(fluoranthene+pyrene)] indicate that combustion processes are the major sources of PAHs. Concentrations of PAHs were poorly correlated with organic carbon concentrations of soils, suggesting different sources and also indicating that the PAH pollution of this area is recent. The same outcome is confirmed by the predominance of PAHs with fewer rings (相似文献   

18.
19.
Yang Y  Ligouis B  Pies C  Achten C  Hofmann T 《Chemosphere》2008,71(11):2158-2167
Organic petrographic analysis was applied to provide direct information on carbonaceous geosorbents for PAHs in river floodplain soils. The anthropogenic OM group (primarily coal and coal-derived particles) displayed large volume amounts for all the soil samples. Distinct PAH concentrations with similar PAH distribution patterns were determined in grain size and density fractions for each sample. Two-ring PAHs had stronger correlation to organic carbon (OC) than black carbon (BC) contents, while heavier PAHs showed correlation to BC, rather than OC. In this study, we combined grain size and density separation, PAH determinations, TOC and BC measurements, and organic petrographic identification, and concluded that two-ring PAHs in soils were associated to coal particles. Other heavier PAHs could be more controlled by black carbon (BC), which were mostly coal-derived particles from former coal mining and coal industrial activity.  相似文献   

20.
This paper presents the first attempt to quantify the production, cycling, storage and loss of PAHs in the UK environment. Over 53 000 tonnes of sigmaPAHs (sum of 12 individual compounds) are estimated to reside in the contemporary UK environment, with soil being the major repository. If soils at contaminated sites are included, this estimate increases dramatically. Emission of PAHs to the UK atmosphere from primary combustion sources are estimated to be greater than 1000 tonnes sigmaPAHs per annum, with over 95% coming from domestic coal combustion, unregulated fires and vehicle emissions. It is estimated that approximately 210 tonnes of sigmaPAH are delivered to terrestrial surfaces each year via atmospheric deposition. Therefore, inputs of PAHs to the UK atmosphere outweigh the outputs by a factor of over 4. This may be explained by enhanced particulate deposition near point sources, PAH degradation in the atmosphere and transport away from the UK with prevailing winds. Disposal of waste residues is estimated to contribute a further 1000 tonnes of sigmaPAH per year to the terrestrial environment. It is illustrated that the use of creosote has the potential to release considerable quantities of PAHs to the UK environment. Temporal trends in PAH cycling are then considered. There is good evidence to suggest that air concentrations and fluxes to the UK surface are now lower than at any time throughout this century. Nonetheless, the UK sigmaPAH burden is still increasing at the present time, principally through retention by soils. However, there are marked differences in the behaviour of individual compounds: there is evidence, for example, that phenanthrene concentrations in soils have declined since the 1960s, although soil concentrations of benzo[a]pyrene and other heavier PAHs have continued to increase through this century. Volatilisation of low molecular weight PAHs accumulated in soils over previous decades may be making an important contribution to the current atmospheric burden. The major uncertainties identified by data on this budget are: (1) the lack of PAH concentrations in some environmental matrices; (2) the possible importance of contaminated soils as a major repository and source of PAHs; (3) the lack of emission data (especially vapour phase releases) for some PAH sources; (4) the importance of biodegradation and volatilisation as loss mechanisms for low molecular weight PAHs in soils; and (5) the importance of creosote use in the PAH cycle.  相似文献   

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