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1.
Aim and Background  Little data are available on the levels of polycyclic aromatic hydrocarbons (PAHs) in the sediments of the Mediterranean Sea Coast of Egypt in general and the Alexandria coastal zone in particular. It was therefore deemed necessary to set up a monitoring programme to determine the current concentrations of PAHs in bottom sediments, and to identify any area where high concentrations of these potential hazardous contaminants were present in the Western Harbour of Alexandria. Methods  The composition, distribution and the source of PAHs in surficial sediments of the harbour were investigated. To document the spatial PAH input, surficial sediment samples from 23 locations throughout the harbour were analysed. as]Results and Discussion The total PAH load determined in the surficial sediment samples ranged from 8 to 131150 ng g1 dry wt, generally with most of the samples having total concentrations of PAHs greater than 5000 ng g1 dry weight. The highest concentration of total PAHs was recorded in sediments of the inner harbour. Ratio values of specific compounds such as phenanthrene to anthracene, fluoranthrene to pyrene, methyl-phen-anthrene to phenanthrene, methyl-dibenzothiophenes to dibenzothiophenes, alkylated to non-alkylated and high molecular weight to low molecular weight PAH, were calculated to evaluate the possible source of PAH contamination in the harbour sediments. Conclusions  Two main sources of PAH in the study area have been found: pyrolytic and petrogenic. Interferences of rather petrogenic and pyrolytic PAH contaminations were noticed for most samples. The dominant sources of PAH appear to be the combustion processes through run-off, industrial and sewage discharges, and atmospheric input. The concentrations of PAHs were generally above levels expected to cause adverse biological effects. Recommendations and outlook  Information from this study and any other relevant studies should be useful in designing future strategies for environmental protection and management of the harbour.  相似文献   

2.

Purpose

The purpose of this study was to elucidate historical trends, spatial variations, and the sources of polycyclic aromatic hydrocarbons (PAHs) pollution in several Japanese lakes.

Materials and methods

The vertical distributions of PAHs in the core samples of sediments taken at several points in lakes Kasumigaura, Suwa, Kizaki, and Shinji were determined using a gas chromatograph equipped with a mass selective detector and combined with chronological information and the physical/elemental properties of the sediment.

Results and discussion

Seventeen related compounds (congeners) typically had concentration peaks at sediment depths corresponding to the 1960s to 1970s. In Lake Shinji and one bay of Lake Kasumigaura, there was a tendency for PAH concentrations to increase downstream; in contrast, another bay of Lake Kasumigaura showed the reverse trend. During big flood events, the fluxes of PAHs increased due to large inputs of particulate matter, although PAH concentrations were reduced. For the four study lakes and other similar lakes, PAH concentrations of surface sediments were approximately proportional to population densities in the respective watersheds, while the total input of PAHs to the lakes were correlated with their population and watershed area. The source apportionment analysis using isomer ratios for the congener profiles indicated that the principal sources of the PAHs in the lake sediments were gasoline and/or diesel engine exhausts and biomass burning.

Conclusions

The observed concentration peaks showed a deterioration of the chemical quality of atmospheric conditions around 1960?C1970 and a recent tendency for their amelioration. Between-lake differences suggest that the influence of human activity in the watersheds influences sediment PAH concentrations. The PAH sources were identified to be of pyrogenic origin.  相似文献   

3.
Background, aims, and scope  Sediments and soils in coastal areas are frequently polluted by anthropogenic contaminants as the result of both riverine or terrestrial discharge and autochthonic marine emissions. In order to determine petrogenic contamination in the coastal industrial area of Kavala City in northern Greece, a combination of polycyclic aromatic hydrocarbon (PAH) and organic geochemical petroleum biomarker analyses has been performed on marine and freshwater sediments as well as soils. Materials and methods  Soils, freshwater, and marine sediments have been treated by standard extraction methods. The dried and desulphurized sample extracts have been fractionated by column chromatography, followed by addition of surrogate standards. Qualitative and quantitative data were obtained by gas chromatograph connected with a flame ionization and electron capture detector (GC-FID/ECD) and by GC linked to a mass spectrometer (GC/MS), whereas identification of compounds was based on EI+-mass spectra and gas chromatographic retention times. Quantitative data were obtained by integration of specific ion chromatograms. Results  The total PAH concentrations measured in the area varied highly, showing different levels from 18 up to 318,000 ng g−1 dry weight (dw). Several PAH ratios, as well as the ratio of pristane (Pr) to phytane (Phyt), have been considered. Out of 39 samples, 22 revealed a specific distribution of hopane fingerprints indicating petrogenic input. Finally, in numerous samples, the ratio of 17α(H)-22,29,30-trisnorhopane (Tm) and 18α(H)-22,29,30-trisnorhopane (Ts) was calculated, as well as the ratio of 22S-17α(H),21β(H)-30 homohopane (αβC31-hopane 22S) and 22R-17α(H),21β(H)-30 homohopane (αβC31-hopane 22R). Discussion  Based on the specific PAH ratios, a group of samples was clearly characterized to be contaminated dominantly by combustion-derived emissions, whereas a second group of samples exhibited mixed influence from petrogenic and pyrogenic PAHs. On the other hand, the exhibition of specific hopane fingerprints in many samples indicates a direct petrogenic input. Finally, the values of the ratio of Tm/(Ts + Tm) and of αβC31-hopanes 22S/(22S+22R)-isomer demonstrated an input of highly mature organic matter that has to be clearly attributed to petroleum-derived contamination, while the ratio of Pr/Phyt showed that most samples exhibited an input of organic matter. Conclusions  The coastal area of Kavala is strongly affected by anthropogenic contaminants. Petrogenic emissions were pointed out firstly by PAH analyses that separated dominantly pyrogenic contaminated sites from areas affected by both pyrogenic and petrogenic emissions. However, analyses of organic geochemical biomarkers revealed a much higher sensitivity in identifying petroleum-derived contaminations and were successfully used to differentiate several petrogenic contaminations in the marine and terrestrial samples. Recommendations and perspectives  Based on this study, it was recommended to use a complementary approach of source-specific substances to successfully characterize petrogenic emissions. Generally, a PAH-based source identification of petrogenic versus pyrogenic contaminations should be combined with petroleum biomarker analysis. PAH and biomarker ratios as well as individual biomarker fingerprints revealed a more comprehensive view on the quality and quantity of petrogenic emissions in sediments and soils.  相似文献   

4.

Purpose

Understanding the fate and behavior of polycyclic aromatic hydrocarbon (PAH) sources in aquatic systems is important for the efficiency of control policies. In this work, a new approach??organic carbon-normalized sediment?Cpore water partition coefficients of PAH source contributions (logK??Osource)??was developed to study the sediment?Cpore water partition of PAH source contributions. The focus of this study was the Yellow River, which is the second largest river in China and one of the largest rivers in the world.

Materials and methods

Sixteen priority US Environmental Protection Agency PAHs were analyzed in 14 surface sediments and 11 pore water samples. Principal component analysis?Cmultiple linear regression (PCA-MLR) and Unmix models were employed to estimate the source contributions of PAHs in sediments and pore water samples. Finally, logK??Osource values were calculated according to the modeled source contributions of PAHs.

Results and discussion

??PAHs (sum of the 16 PAH concentrations) in 14 sediment samples and 11 pore water samples from the Yellow River were 1,415?±?726?ng?g?1 dry weight (dw) and 123?±?57.4???g?l?1, respectively. The source apportionment results indicate the following: (1) for sediment samples, the contributions to ??PAHs from vehicular emissions, coal combustion, and petrogenic sources were 41.07?C61.05, 38.83?C45.56, and 11.18?C14.92?%, respectively, and (2) for pore water samples, vehicular emissions were the most significant contributor (45.51?C69.39?%), followed by petrogenic sources (29.80?C34.22?%) and coal combustion (7.35?C21.59?%). Coal combustion had the highest logK??Osource values (4.15?C4.26) among the three categories, followed by vehicular emissions (3.51?C3.57) and petrogenic sources (3.30?C3.43).

Conclusions

The possible categories of PAH sources identified by hierarchical cluster analysis, PCA-MLR, and Unmix models were consistent, indicating that vehicular emissions, coal combustion, and petrogenic sources were three important categories. The logK??Osource values indicate that contributions from coal combustion had a higher partition for the sediment phase compared with the other two source categories.  相似文献   

5.
Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous toxic organic pollutants in the natural environment that are strongly associated with socioeconomic activities. Exploring the distribution, sources, and ecological toxicity of PAHs is essential to abate their pollution and biological risks. The 16 priority PAHs in different lakeside city estuarine sediments in the northern Taihu Lake in China were determined using gas chromatography-mass spectrometry. Results showed that total concentrations...  相似文献   

6.

Purpose

Obtaining a better understanding of the concentrations and origins of polycyclic aromatic hydrocarbons (PAHs) in the sediments Taihu Lake, China, is of paramount importance for the environmental protection and remediation of this lake. To investigate temporal and spatial variations in PAH concentrations, composition and possible source categories, 29 sediment samples were collected from Taihu Lake during both the flooding and dry seasons of the lake.

Materials and methods

Fifteen US Environmental Protection Agency priority PAHs were detected in 58 surface sediments (29 for each season) by gas chromatograph/mass selective detection, following extraction by accelerated solvent extraction.

Results and discussion

The concentrations of the total and individual PAHs in the flooding season were higher than those in the dry season, suggesting that high levels of fishing activity may be an important contributor to PAH pollution in the flooding season. The fractions of high molecular weight PAHs in the flooding season ranged from 63?% to 71?% and were higher than those in the dry season (which ranged from 52?% to 65?%). These results indicate that vehicle exhaust may be a more important pollutant source in the flooding season than in the dry season. Diagnostic ratios, principal component analysis and hierarchical cluster analysis were used to study possible source categories in the different seasons. Consistent results were obtained for all techniques. Seasonal and spatial variations were also investigated by the coefficient of divergence method. The results of previous studies support the conclusion of source identification.

Conclusions

Vehicle emissions were the dominant contributor to PAHs in the flooding season, while PAHs in the dry season sediments may have come from multiple sources. The findings of this study may provide a theoretical basis for seasonal PAH control strategies for Taihu Lake.  相似文献   

7.
Pine needles were selected as cost-effective and easy collectable matrices suitable for long-term monitoring of the lower troposphere pollution with polycyclic aromatic hydrocarbons (PAHs). Overall, 27 sampling sites around the island of Crete were selected, and upon availability, second- and third-year needles from two pine species (Pinus brutia Ten. and Pinus pinea L.) were collected. In general, the results for both pine species showed that sites belonging in the urban group yielded the highest contamination levels when compared to the rural and the remote ones and that third-year needles had higher PAH contamination than the second-year ones. Phenanthrene was the prevailing PAH, representing 39% and 46% of the total contamination for second- and third-year needles, respectively. Fluoranthene, pyrene, chrysene and fluorene followed, with individual concentrations between 6% and 12%. The dominance of three-ringed PAHs was evidenced for the vast majority of the sites. An urban, rural and remote fingerprint was determined over a more general uniform contamination pattern, and the diagnostic PAH ratios pointed towards mixed petrogenic and pyrogenic sources. Overall, the present findings showed that the presence of PAHs is not negligible throughout the Cretan atmosphere and can be even considered quite high in some areas, especially when comparing the results to the ones found for more densely populated or industry-related areas.  相似文献   

8.
Background, Aim and Scope  Polycyclic aromatic hydrocarbons (PAHs) have gained serious attention in the scientific community due to their persistence and toxic potential in the environment. PAHs may pose a risk to ecosystem health. Along the Mosel River/Germany, a tributary of the river Rhine, PAHs were found at significantly high concentrations (> 20 mg kg−1, German national guideline value Z2, LAGA 1998). These high concentrations were detected during the construction of a storm water retention basin, in which the contaminated soils had to be removed and treated as hazardous waste. This resulted in higher construction costs for implementing flood prevention measures, but did not address the origin of these PAHs and its distribution along Mosel River. Hence, for future flood prevention projects, it is necessary to estimate the extent of PAH contamination along the Mosel River. The aim of the study is to determine the extent of PAH contamination in soils collected along Mosel and Saar River, and to obtain a first insight into the origin of the PAH contamination in this region. Materials and Methods  In total twenty seven sample sites were investigated. Forty two single samples were collected along a 167 km distance of Mosel River and six samples were collected along a 20 km distance of Saar River. Soil samples were collected at a depth of 0 to 2 m with a stainless steel corer (▫ 8 cm). Each 2 m sample was further separated into two sub-samples (0–1 m and 1–2 m). The sixteen EPA PAHs and three additional PAHs (1methylnaphthalene, 2methylnaphthalene and perylene) were analysed with gas chromatography mass spectrometry (GC-MS). For soil characterisation, total organic carbon (TOC), grain size, microscope and X-ray diffraction (XRD) analysis were performed. Results  Grain size for all soil samples was classified as a mixture of sand and silt. XRD analysis showed that all samples were dominated by quartz. Some clay minerals, such as illite and montmorillonite and feldspars, i.e. anorthoclase and orthoclase, were found in minor quantities. TOC ranged from 0.1% to 13%. Microscope analysis showed black coal particles in the majority of the soils collected from the Saar River and part of the Mosel River (downstream of the confluence of Saar and Mosel River). The black particles were not found further upstream along Mosel River. The sum of nineteen PAHs in the soil samples was up to 81 mg kg−1 dry weight (dw). Most soil samples showed a relationship between the presence of coal particles and PAH concentrations. Discussion  Elevated PAH concentrations were found in all soil samples collected from Saar River and downstream Mosel River. Due to former coal mining activities in the Saarland, Germany, there is a strong evidence that the majority of the PAH contamination in the soils downstream Mosel River are linked to these mining activities. Upstream Mosel River coal particles were hardly found although PAH concentrations were high. Therefore another PAH source has to be responsible for these concentrations. PAH distribution patterns indicate a pyrogenic PAH input upstream Mosel River and a mixed input (petrogenic and pyrogenic) downstream Mosel River. Conclusions  Due to PAH distribution patterns, the contamination along the upstream of the Mosel River is probably linked to atmospheric depositions and other sources not linked to coal mining activities. Downstream Mosel River the PAH distribution patterns reflect former coal mining activities. We could corroborate for the first time that coal mining resulted in a serious problem of an extensive PAH contamination at Saar and Mosel River floodplain soils. Recommendations and Perspectives  Coal mining activities have a strong impact on the neighbouring regions (Johnson and Bustin 2006, Short et al. 1999, Stout et al. 2002). It is known that coals exhibit relative high PAH concentrations, especially in the low molecular weight PAHs (Chapman et al. 1996, Radke et al. 1990). However, PAHs in coals are hardly bioavailable (Chapman et al. 1996) and hence may have less adverse effects on exposed biota. They can act as sink for other hydrophobic contaminants. For the assessment of the environmental impact, a detailed study of the sorption and desorption behaviour of PAHs linked to coal particles should be carried out. ESS-Submission Editor: Dr. Ralph Portier (rportie@lsu.edu)  相似文献   

9.
Polycyclic aromatic hydrocarbons (PAHs) can enter the marine environment from a variety of anthropogenic sources. As some PAHs are known or suspected carcinogens and mutagens, their potential hazard to human health and the natural environment warrants investigation. This is the first reported study on the prevalence and concentration of PAHs in marine sediments from Singapore's coastal environment, and accompanies the report by Basheer et al. (2003) on the measurement of persistent organic pollutants (POPs) in seawater. The concentration of 16 PAH, classified as USEPA priority pollutants were analysed in sediments from 22 sample stations located within the northeastern and southwestern regions of Singapore's marine waters. The total PAH concentration varied between 15.22 μg g-1 and 82.41 μg g-1 in the northeastern region and between 13.63 μg g-1 and 84.92 μg g-1in the southwestern region. The highest concentration of total PAH i.e. 84.92 μg g-1 was recorded at a site adjacent to a petrochemical refinery. Among the sixteen individual PAHs, chrysene, indeno[1,2,3-cd]pyrene and benzo[a]anthracene were most prevalent in the sediments. The relatively low kinetic/thermodynamic isomer ratios for PAHs suggest that PAHs of pyrogenic origin are predominant in Singapore's coastal environment. The distribution of higher molecular weight i.e. (4–5 ring) individual PAHs corresponded to mixture profiles typical of those originating from high temperature combustion processes subjected to photolytic degradation during long-range atmospheric transportation. A comparison of total PAH concentration data for sediments collected from Singapore relative to those reported for other countries indicates a moderate level of PAH contamination in Singapore's coastal marine sediments.  相似文献   

10.
Studies aimed at determining the deposition history of energy related, potentially carcinogenic, polycyclic aromatic hydrocarbons (PAHs) deposited in the sediments of Cayuga Lake, in the Finger Lakes Region of central New York State, are described. PAH fluxes in the 1850's were at least an order of magnitude less than the maximum rates in the period of 1940 to 1955. PAH fluxes began to decline before the Milliken coal fired power plant, located on Cayuga Lake, started service in 1955. Correlation between the PAH flux into the sediments and fossil fuel usage and emissions for the states of New York, Ohio and Pennsylvania and the United States as a whole, suggests that modern, high efficiency fossil fuel fired power plants are minor sources of PAHs compared to coal related residential heating and industrial combustion. Similar comparisons with historic emissions data do not support the hypothesis that PAH flux is a useful indicator of the combustion sources which produce the `acidifying' compounds SO2 and NOx for the Finger Lakes region.  相似文献   

11.
The concentration of polycyclic aromatic hydrocarbons (PAHs) was determined in seawater, sediment, and Rock oyster Saccostrea cucullata collected from four sampling sites in the inter-tidal areas of Bushehr province. The total concentrations of 14 PAHs varied from 1.5 to 3.6 ng/L in seawater, 41.7 to 227.5 ng/g dry weight in surface sediment, and 126 to 226.1 ng/g dry weight in oyster tissue. In comparing PAH concentrations among the three matrices in Bushehr province, data showed that the pattern of individual PAHs in seawater, oyster, and sediment were different. The oysters tended to accumulate the lower molecular weight and the more water-soluble PAHs. Sediment samples were distinguished from the sea water and oyster samples by the presence of high molecular weight PAHs, especially six-ring PAHs. Three- and four-ring PAHs were the most abundant compounds among the 14 PAHs investigated in surface seawater, sediment, and oyster samples. As expected, differences in octanol/water partition coefficient among individual PAHs and the greater persistence of the higher molecular weight PAHs contributed to the accumulation patterns in oyster and sediment. The results of the study suggested that the main sources of PAHs in the seawater and sediment in the region were mixed pyrolitic and petrogenic inputs.  相似文献   

12.
Polycyclic aromatic hydrocarbons (PAHs) are widespread environmental pollutants produced by incomplete combustion sources such as home heating, biomass burning, and vehicle emissions. PAH concentrations in soils are influenced by source inputs and environmental factors that control loss processes and soil retention. Many studies have found higher concentrations of these pollutants in soils within cities of temperate climates that have a centralized urban core. Less is known about the factors regulating PAH abundance in warm, arid urban ecosystems with low population densities but high traffic volumes. The relative importance of sources such as motor vehicle traffic load and aridland ecosystem characteristics, including temperature, silt, and soil organic matter (SOM) were explored as factors regulating PAH concentrations in soils near highways across the metropolitan area of Phoenix, AZ (USA). Highway traffic is high compared with other cities, with an average of 155,000 vehicles/day. Soils contained low but variable amounts of SOM (median 2.8?±?1.8% standard deviation). Across the city, median PAH concentrations in soil were low relative to other cities, 523?±?1,886 ??g/kg, ranging from 67 to 10,117 ??g/kg. Diagnostic ratio analyses confirmed that the source of PAHs is predominantly fuel combustion (i.e., vehicle emissions) rather than petrogenic, biogenic, or other combustion sources (coal, wood burning). However, in a multiple regression analysis including traffic characteristics and soil properties, SOM content was the variable most strongly related to PAH concentrations. Our research suggests that dryland soil characteristics play an important role in the retention of PAH compounds in soils of arid cities.  相似文献   

13.
Background, aim, and scope  Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous environmental pollutants. They are formed during pyrogenic and diagenetic processes and are components of petrogenic materials such as oils and coals. To identify PAH sources, several studies have employed forensic methods, which may be costly to execute. Although a large number of possible forensic methods are available (e.g., total ion chromatograms, PAH ratios, PAH alkyl homologue series, isoalkanes and isoprenoids, steranes and terpanes, stable isotope ratios, n-alkanes), one has to decide which method is the appropriate cost effective screening approach. In this study, three approaches were tested and compared by measuring (1) an extended PAH spectrum (i.e., 45 instead of the common 16 EPA-PAHs), (2) PAH ratios and (3) n-alkanes to determine if point sources are distinguishable from non-point sources, and if an individual source can be distinguished from a multiple source contaminated site in the study area. In addition, the study evaluated whether these methods are sufficient for source identification of selected samples, and if they constitute a sound strategy for source identification prior to the selection of more cost intensive methods. Materials and methods  Eighteen samples with previously characterized PAH point sources (previously characterized point sources in the Mosel and Saar region) were analyzed. Additionally, three river bank soils of Mosel and Saar rivers with known non-point PAH sources were investigated. The point sources were two gasworks, a tar impregnation facility, a creosoted timber, an acid tar, a tank farm, and a diesel contaminated site. Non-point sources were hard coal particles and atmospheric inputs in river bank soils. All samples were extracted with hexane and acetone, analyzed with a gas chromatograph coupled to a mass spectrometer for PAH distribution patterns and ratios. n-Alkanes were measured by a gas chromatograph equipped with a flame ionization detector. Results  Samples collected from point sources and non-point sources were analyzed by the use of three forensic methods, i.e., PAH patterns of an extended PAH spectrum, PAH ratios and n-alkanes. Identification by PAH patterns alone was insufficient for the non-point sources and some point sources, since the n-alkanes must be measured, as well. The use of PAH ratios with only 16 EPA-PAHs is less indicative in determining multiple sources because source assignments (or categories) change depending on the ratio used. Discussion  This study showed that by employing an extended PAH spectrum it is possible to fingerprint and distinguish sources. The use of alkylated PAHs is essential for identifying petrogenic sources. It is insufficient to rely exclusively on either the common 16 EPA-PAHs or the ratios to the parent PAHs when identifying non-point sources. Source identification using PAH ratios is only reliable if both parent and alkylated PAHs are measured. n-Alkane analyses provide more detailed information about petrogenic sources by verifying the presence of oils, diesel, gasoline, or coal in non-point sources. Conclusions  The three methods tested were deemed sufficient to distinguish between point and non-point PAH sources in the samples investigated. The use of an extended PAH spectrum provides the first step toward identifying possible sources. It simplifies the decision whether additional forensic methods should be necessary for more detailed source identification. Recommendations and perspectives  The determination of PAH alkyl homologue series, biomarkers, and isotopes is often advised (Kaplan et al., Environ Forensics 2:231–248, 2001; Oros and Simoneit, Fuel 79:515–536, 2000; Wang and Fingas, Mar Pollut Bull 47:423–452, 2003). The methods involved are complex and often expensive. We recommend a relatively uncomplicated and cost-effective method (i.e., extended PAH spectrum) before further and more expensive forensic investigations are to be conducted. Additional research with an extended sample set should be carried out to validate these findings for other sources and sites. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.  相似文献   

14.

Goal, Scope and Background

Distribution of hydrophobic organic contaminants in abiotic compartments is essential for describing their transfer and fate in aquatic ecosystems. Taihu Lake is the third largest freshwater lake in China. Water quality of Taihu Lake has deteriorated greatly during the last decades and has threatened the water supply. The aim of the present study was to investigate the partitioning of polycyclic aromatic hydrocarbons (PAHs) among overlying water, suspended particulate matter (SPM), sediments, and pore water in Meiliang Bay, Taihu Lake and to provide useful information for the ecological engineering in this area.

Materials and Methods

Overlying water and surface sediment were sampled from six sites in Meiliang Bay, Taihu Lake, China. Within 72 h of sampling, sediments were centrifuged to obtain the pore water. Overlying water samples were filtered to separate dissolved and SPM samples. After extraction, samples were purified following a clean-up procedure. PAH fraction was obtained by elution with a mixture of hexane: DCM (7:3, V/V) and analyzed by GC/MS.

Results

PAHs concentrations in overlying water varied from 37.5 ng/L to 183.5 ng/L. Concentrations of PAHs in pore water were higher than those in overlying water. The total concentrations of 16 priority PAHs in sediments ranged from 2091.8 ng/g-dw to 4094.4 ng/g-dw. PAHs concentrations on SPM were decreased with suspended solid concentrations (SSC). Total PAHs concentrations on SPM varied in the range of 3369.6 ng/g-dw to 7531.1 ng/g-dw. The partition coefficients between sediment and overlying water (log K oc) for PAHs with log K ow<5 were positively correlated with their octanol-water partition coefficients (log K ow) (n=39, r=0.79, p<0.0001). Partition coefficients between sediment and pore water (log K oc′) for all PAHs were also significantly correlated with their log K ow values (n=48, r=0.82, p<0.0001).

Discussion

In general, PAHs derived from combustion sources tend to bind strongly to soot particles in natural sediment. Consequentially, K oc values observed in the natural environment could be orders of magnitude higher than those predicted by linear correlation relationships under laboratory conditions. In the present study, the ratio of log K oc values to log K ow values falls consistently above 1, indicating that the sediment soot carbon in the bay was more attractive for PAHs than n-octanol. The log K oc′ was also higher than that predicted under laboratory conditions, suggesting that the measured pore water PAH concentrations were lower than those predicted. That is to say, not all the sediment PAHs can be available to partition rapidly into sediment pore waters. A variation in soot content is a possible reason. Furthermore, concentrations of PAHs on SPM were higher than those in sediments. The compositions of PAHs on SPM and in sediments were similar, indicating the importance of re-suspension process of sediments in the partitioning process of the shallow lake.

Conclusions

The results indicated the equilibrium partitioning model could be used to predict PAHs distribution in various phases of a shallow lake in the stagnation period, but re-suspension processes should be considered to modify the relationship between log K ocs and log K ows.

Recommendations and Perspectives

Concentration, particle size and composition of resuspended particles could affect the relationship between log K ocs and log K ows. Further work should be done under field conditions, especially where a steady thermodynamic equilibrium state could be assumed.
  相似文献   

15.
Intention, Goal, Scope, Background  Environmental pollution caused by oil spills is a major ecological problem. Oil contamination in the environment is primarily evaluated by measuring the chemical concentrations of hydrocarbons. The results of chemical analyses are important for estimating water and sediment quality in the risk assessment to the flora and fauna of oil-contaminated sites. In the world there are lake ecosystems under permanent chemical stress due to urbanization and the oil industry. Studies, however, have been generally limited to petroleum compounds and have not considered other pollutants of the site like PCBs, polychlorinated pesticides and heavy metals. Objective  Water and sediment from stations in the Mecoacán Lake in the Mexican State of Tabasco were analyzed for polycy-clic aromatic compounds (PAHs), aliphatic hydrocarbons (AHs), polychlorinated biphenyls (PCBs), polychlorinated pesticides (PCPs) and heavy metals. The objective of this study was to examine the contaminant levels of the samples collected in February 1993 and 1996 after oil spills at the Mecoacán petroleum region. The goals of this study were to reveal the effect of the spills on the distribution of the hydrocarbons and assess the toxi-cological significance of the levels found. In addition, our aim was to examine the distribution of the PAHs in sediments from Mecoacán originated from both pyrolytic and petrogenic sources. Methods  Samples were collected from 19 stations and prepared according to the CARIPOL (Caribbean Pollution) methodology of the United Nations Environmental Programme (1992) of the Great Caribbean Region for hydrocarbons in marine and coastal water, and sediments. The gas-chromatographic and atomic absorption analysis of the samples was performed after sampling. Results and Discussion  Concentrations of PAHs in water ranged from 0.2 to 0.8 μg/l in 1993 and from 0.3 to 2.8 μg/l in 1996. The concentration of the 16 EPA-PAHs varied from 0.1 to 36 mg/kg dry weight in the lake sediment samples collected in 1996, while those of AHs, PCBs and PCPs ranged from 0.1 to 67 mg/kg, 0.1 to 59 μg/kg and 6 to 370 μg/kg, respectively. The most abundant contaminants in water were benz[a]anthracene and pyrene, in 1993 and 1996, respectively; while in sediments collected in 1996: Pyrene, C24, 2-chlorobiphenyl and endrin predominated. Heavy metals (Cu, Pb and Zn) were found at low concentrations. Benzo[a]pyrene was detected in some sediment samples in varying amounts (0.2 to 0.3 mg/kg). Conclusions  The maximum total PAH concentration in sediments was found at sites near the oil fields and the AH concentration near the urban zone. The mayor pollutants in sediments were PAHs and AHs, and taking into regard the detected PAHs near the oil fields, the source was the oil spilling. The mean total PAH value in Mecoacan sediments of 6.4 mg/kg did not exceed the median range effects value (ERM) for total PAHs of 44.8 mg/kg. The measured organochlorine compounds and heavy metals were present in amounts much inferior to the ERM values. This study confirms that contaminants concentration in sediments did not exceed the environmental quality guideline for the 50% probability and no adverse effect can be expected. Recommendation and Outlook  Analysis revealed no indication of a contribution of PAHs, PCBs, PCPs and heavy metals to acute sediment toxicity. The results of this study demonstrate the importance of continuous monitoring of ecosystems exposed to pollution to make pre-spill data available in order to evaluate the real consequence of the spilling and its effect on flora and fauna.  相似文献   

16.
The accumulation features of pyrogenic polycyclic aromatic hydrocarbons (PAHs) in soils were analyzed depending on the type of burning material and the combustion conditions (the temperature, oxygen access, and dispersion of the combustion products). The PAH accumulation features in the soils of three reserved areas of forest, steppe, and peat fires were revealed. The distribution features of the PAHs resulting from the anthropogenic pyrogenic processes (the household combustion of wood and the inflammation of coal dumps) in soils were established. The differences in the qualitative composition of the PAHs arriving to the soils from the different pyrogenic sources were shown.  相似文献   

17.
Pun  K. L.  Law  Shuen  Li  Gang 《Journal of Soils and Sediments》2019,19(2):973-988
Purpose

This study investigated the concentrations of cadmium (Cd), chromium (Cr), copper (Cu), lead (Pb), nickel (Ni), zinc (Zn), and polycyclic aromatic hydrocarbons (PAHs) in sediments collected from gully pots for road drainage in Hong Kong. The presence and intensity of anthropogenic contamination of road gully sediments were assessed. Identifications of potential sources of trace elements and PAHs were performed to help understand the situation for future control of pollution to the land and aquatic environments.

Materials and methods

Gully sediment samples were collected from gully pots of 18 roads that are potentially exposed to different pollution sources in Hong Kong. The selection of roads considered different road features, adjacent land uses, and traffic volumes. Composite samples were collected for the analysis of trace elements (Cd, Cr, Cu, Pb, Ni, and Zn) and PAHs by an accredited environmental testing laboratory. Geo-accumulation index (Igeo), contamination factor (Cf), modified degree of contamination (mCd), ecological risk factor (Er), and pollution load index (PLI) were used to assess the level of ecological risk of trace element contamination. Positive matrix factorization (PMF) and PAH diagnostic ratios were applied to identify the sources of trace elements and PAHs.

Results and discussion

Elevated trace element concentrations were commonly found in gully sediments. The concentrations of Zn (267–3700 mg kg?1) were the highest compared to the other trace elements. Noticeable high concentrations of Cu (27–1020 mg kg?1), Pb (21–332 mg kg?1), and Cr (14–439 mg kg?1) were found in all samples. The PAH contents were moderate to high (0.6 to 24.7 mg kg?1). Commercial/industrial emissions and road features that cause frequent acceleration-deceleration and turning events showed important influences on the contaminant levels. Strong correlations between the concentrations of Cd, Cr, Pb, and Zn were identified, implying that these trace elements are likely from common sources. The contamination assessment indices reflect significant sediment pollution. The ecological risk ranges from the considerable/moderate-risk class to over the high-risk class.

Conclusions

The collected gully sediments are identified as highly contaminated and need to be isolated from the environment upon final disposal. Through the comprehensive analysis of the collected data, this study provides a detailed insight into the contaminant levels of road gully sediments and potential sources of contamination. Disposal of gully sediments and potential impacts due to release of contaminants into the downstream aquatic environment during rainstorm events should receive attention and need further investigation.

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18.
PAHs are mainly produced by combustion processes and consist of a number of toxic compounds. While the concentrations of individual PAHs in soil produced by natural processes (e.g., vegetation fires, volcanic exhalations) are estimated to be around 1—10 μg kg−1, recently measured lowest concentrations are frequently 10 times higher. Organic horizons of forest soils and urban soils may even reach individual PAH concentrations of several 100 μg kg−1. The PAH mixture in temperate soils is often dominated by benzofluoranthenes, chrysene, and fluoranthene. The few existing studies on tropical soils indicate that the PAH concentrations are relatively lower than in temperate soils for most compounds except for naphthalene, phenanthrene, and perylene suggesting the presence of unidentified PAH sources. PAHs accumulate in C‐rich topsoils, in the stemfoot area, at aggregate surfaces, and in the fine‐textured particle fractions, particularly the silt fraction. PAHs are mainly associated with soil organic matter (SOM) and soot‐like C. Although the water‐solubility of PAHs is low, they are encountered in the subsoil suggesting that they are transported in association with dissolved organic matter (DOM). The uptake of PAHs by plants is small. Most PAHs detected in plant tissue are from atmospheric deposition. However, earthworms bioaccumulate considerable amounts of PAHs in short periods. The reviewed work illustrates that there is a paucity of data on the global distribution of PAHs, particularly with respect to tropical and southern hemispheric regions. Reliable methods to characterize bioavailable PAH pools in soil still need to be developed.  相似文献   

19.

Purpose

The choice and timing of microorganisms added to soils for bioremediation is affected by the dominant bioavailable contaminants in the soil. However, changes to the concentration of bioavailable PAHs in soil are not clear, especially when several PAHs coexist. This study investigated the effects of PAH concentration and chemical properties on desorption in meadow brown soil after a 1-year aging period, which could reflect changes of PAH bioavailability during bioremediation.

Materials and methods

Based on the percentage of different molecular weights in a field investigation, high-level contaminated soil (HCS) and low-level contaminated soil (LCS) were prepared by adding phenanthrene (PHE), pyrene (PYR) and benzo(a)pyrene (BaP) to uncontaminated meadow brown soil. The concentrations of HCS and LCS were 250 mg?kg?1 (PHE, PYR, and BaP: 100, 100, and 50 mg?kg?1) and 50 mg?kg?1 (PHE, PYR, and BaP: 20, 20, and 10 mg?kg?1) respectively. The soils were aged for 1 year, after which desorption was induced by means of a XAD-2 adsorption technique over a 96-h period.

Results and discussion

The range of the rapidly desorbing fraction (F rap) for PHE, PYR, and BaP in HCS and LCS was from 1.9 to 27.8 %. In HCS, desorption of PYR was most difficult, and the rate constant of very slow desorption (K vs) of PYR was 8 orders of magnitude lower than that of BaP, which had similar very slow desorbing fractions (49.8 and 50.5 %, respectively). However, in LCS, desorption of PYR was the easiest; the Kvs of PYR was 8–10 orders of magnitude higher than those of PHE and BaP. In HCS, the time scale for release of 50 % of the PAHs was ranked as BaP?>?PYR?>?PHE, while in LCS this was BaP?>?PHE?>?PYR.

Conclusions

The combined effect of PAH concentrations and properties should be taken into account during desorption. The desorption of PAH did not always decrease with increasing molecular weight, and the desorption of four-ring PAHs might be special. These results are useful for screening biodegrading microbes and determining when they should be added to soils based on the dominant contaminants present during different periods, thus improving the efficiency of soil bioremediation.  相似文献   

20.
Background, Aims, and Scope  More frequent occurrence of stronger floods in Europe as well as in other parts of the world in recent years raises major concern about the material damages, but also an important issue of contamination of the affected areas through flooding. The effects of major floods on levels and distribution of contamination with hydrophobic organic pollutants were examined from the continuous set of data for floodplain soils and sediments from a model industrial area in the Czech Republic where a 100-year flood occurred in 1997. The goal of this study was to evaluate the risk related to contamination associated with such extensive natural events and characterize the spatial and temporal distribution and dynamics of pollutants related to a major flooding shortly after the floods and also in the time period several years after floods. Methods  Sediments and alluvial soils from fourteen sites each were repeatedly sampled during the period from 1996 until 2005. The sampling sites represented five regions. Collected top-layer sediment and soil samples were characterized and analyzed for hydrophobic organic pollutants PCBs, OCPs and HCB using GC-ECD and PAHs using a GC-MS instrument. Spatial and temporal differences as well as the relative distribution of the pollutants were examined in detail by statistical analysis including multivariate methods with special emphases placed on the changes related to floods. Results  The organic pollutants levels in both alluvial soils and sediments exceeded the safe environmental limits at numerous sites. Pollutants concentrations and relative distribution as well as organic carbon content in both sediment and floodplain soils were significantly affected by the flooding, which resulted in a decrease of all studied contaminants in sediments and significant rise of the PAH pollution in the flooded soils. There was a unique and highly conserved PAH pattern in soils regardless of the floods and greater changes in PAH pattern in sediments related to floods. The relative distribution of individual PAHs reflected a combustion generated PAH profile. PAH levels in the river sediments rose again at the sites with continuous sources several years after floods. Discussion  The results showed different dynamics of PAHs and PCBs during the floods when PAHs were redistributed from the sediments to alluvial soils while PCBs have been washed out of the study regions. The data reveal longer contamination memory and consistent contamination pattern in soils, whereas sediments showed more dynamic changes responding strongly to the actual situation. The stable PAH pattern within the regions also indicates that a relative amount of all compounds is comparable across the samples and, thus, that the sources at different sites have similar character. Conclusions  Sediments have the potential to function as a secondary source of contamination for the aquatic ecosystem, but also for the floodplain soils and other flooded areas. The floods served as a vector of PAHs contamination from sediments to soils. The reloading of river sediments in time, namely with PAHs, due to present sources increases their risk as a potential source in the next bigger flood event both to the downstream river basin and affected alluvial soils. Recommendations and Perspectives  The results stress the importance of including the floodplain soil contamination in the risk assessment focused on flood effects. Floodplain soils have stable long-term environmental memory related to contamination levels, pattern and distribution, whereby they can provide relevant information on the overall contamination of the area. The sediments will continue to serve as a potential source of contaminants and alluvial soils as the catchment media reflecting the major flood events, especially until effective measures are taken to limit contamination sources. ESS-Submission Editor: Dr. Henner Hollert (Hollert@uni-heidelberg.de) This article is openly accessible!  相似文献   

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