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1.
Thirty-three sediment samples from Hsin-ta Harbour and neighboring coastal areas were analyzed by GC-MS for polycyclic aromatic hydrocarbons (PAHs). Total concentrations of 30 analyzed parental and alkylated PAHs ( summation operator PAH) varied from 98.1 to 3382 ng/g dry weight. MP/P (methylphenanthrenes/phenanthrene) values larger than 2 coincided with very low P/A (phenanthrene/anthracene) values at inner harbour stations, revealing that a significant portion of low molecular weight PAHs are probably from petrogenic pollution sources, specifically, illegal disposal of used motor oil. The 4,6-dimethyldibenzothiophene/3,6-dimethylphenanthrene (4,6-C(2)D/3,6-C(2)P) ratio is found to be more useful than the MP/P ratio in tracing petrogenic PAHs from the inner harbour area to the adjacent coastal environment. In addition, according to hierarchical cluster analysis, collected sediments cluster in three major groups, Off-shore Group, Near-shore Group and Inner Harbour Group. Three diagnostic ratios, 4,6-C(2)D/3,6-C(2)P, PER/ summation operator PAH (perylene to summation operator PAH) and BaA/CHR (benzo(a)anthracene/chrysene), representing petrogenic, biogenic and pyrogenic origins, are found to be effective in differentiating and characterizing sediments among the groups in this study. Enrichment of pyrogenic and petrogenic PAHs in sediments collected exhibits mixing or dilution, spatially, by biogenic (or natural) PAHs.  相似文献   

2.
Development of oil hydrocarbon fingerprinting and identification techniques   总被引：30，自引：0，他引：30  
Oil, refined product, and pyrogenic hydrocarbons are the most frequently discovered contaminants in the environment. To effectively determine the fate of spilled oil in the environment and to successfully identify source(s) of spilled oil and petroleum products is, therefore, extremely important in many oil-related environmental studies and liability cases. This article briefly reviews the recent development of chemical analysis methodologies which are most frequently used in oil spill characterization and identification studies and environmental forensic investigations. The fingerprinting and data interpretation techniques discussed include oil spill identification protocol, tiered analytical approach, generic features and chemical composition of oils, effects of weathering on hydrocarbon fingerprinting, recognition of distribution patterns of petroleum hydrocarbons, oil type screening and differentiation, analysis of “source-specific marker” compounds, determination of diagnostic ratios of specific oil constituents, stable isotopic analysis, application of various statistical and numerical analysis tools, and application of other analytical techniques. The issue of how biogenic and pyrogenic hydrocarbons are distinguished from petrogenic hydrocarbons is also addressed.  相似文献   

3.
The quantitative concentrations of 21 congeners of polychlorinated biphenyls and 16 priority polycyclic aromatic hydrocarbons were studied in bottom sediments of the Usa River, the largest Pechora’s tributary, and its tributaries located in the central part of Timan-Pechora petroleum province. In accordance with the classification of the regional and international standards, the pollution degree of bottom sediments by organic compounds of those classes was evaluated. Pollution profiles were examined and the character of the dominating source of polychlorinated biphenyls and polycyclic aromatic hydrocarbons for bottom sediments in the region under study was identified. Key words: bottom sediments, polychlorinated biphenyls, profiles of polycyclic aromatic hydrocarbons, petrogenic, pyrogenic pollution source.  相似文献   

4.
The distribution of selected hydrocarbons within ten dated sediment cores taken from the Mississippi River Bight off coastal Louisiana suggests a chronic contaminant loading from several sources including the river itself, oil and gas exploration in the central Gulf of Mexico (GOM) shelf area, and natural geologic hydrocarbon seeps. Data were grouped as either total polycyclic aromatic hydrocarbons (PAH's), which were indicative of pyrogenic PAH's; or estimated total hopanes (indicative of petrogenic hydrocarbons). The total PAH concentrations and estimated total hopanes begin increasing above background levels (approximately 200 ng g(-1)) after the 1950s. The distribution of these hydrocarbons and hopanes within the dated sediment cores suggests that the Mississippi River is a regional source of pyrogenic PAH's, and that the hopanes are from natural geologic hydrocarbon seeps, oil and gas exploration in the GOM, or both.  相似文献   

5.
The distribution of aliphatic and aromatic hydrocarbons was determined in surface sediments collected at 36 stations along the Galicia continental shelf (NW Spain), following the Prestige oil spill. Sampling was performed in December 2002, just after the accident, and in February and September 2003. Concentrations of PAHs (summation operator 13 parent components) were in the range of 0.9-422 microg/kgdw, the highest values being close to coastal urban areas (e.g. Pontevedra and A Coru?a), whereas in the stations of the area most heavily impacted by the spill (off Costa da Morte) concentrations were in the range of 14.8-89.6 microg/kgdw, with a certain predominance of alkylated compounds, which may suggest a mixture of petrogenic and pyrolytic sources. The detailed study of petrogenic molecular markers (e.g. steranes and triterpanes) showed the occurrence of an old (weathered) petrogenic chronic pollution in the shelf sediments but not of the Prestige oil, with the possible exception of few stations in the area of Costa da Morte. This was attributed to the heavy nature of the spilled oil that was barely dispersed in the water column and mainly stranded on the coast or sedimented in the form of oil patches. The addition of increasing amounts of fuel oil to a representative sediment sample showed that the molecular indices were indicative of the presence of the Prestige oil when the amount was above 1g/kg of sediment. The toxicity of selected samples (showing the higher PAH concentrations) was tested using the bivalve embryogenesis bioassay. Embryogenesis success reached high values in all cases (80-88%, with 86% in the control), indicating a lack of toxicity in the sediments and supporting the conclusion that the patchiness of the fuel eventually reaching the seafloor reduced its impact on the benthic communities of the Galician shelf.  相似文献   

6.
In this study, we measured and analyzed polycyclic aromatic hydrocarbons (PAHs) in surface sediment samples collected from the Kaoping river and submarine canyon (KPSC) system to determine the compositional patterns and characteristic distributions of PAH and to elucidate the transport and fate of these land-derived particles. Concentrations of total PAH (sum of 28 PAH compounds) ranged from 22.6 to 45,100 ngg(-1) dry weight (dw) and the highest concentrations were found in the sediments of Donggang Harbor. The ratio of perylene to sum of penta-aromatic PAH isomers (47-55%) was higher in off-shore stations, suggesting a diagenetic PAH source. Various isomeric ratios also indicated that combustion was a significant source of PAH to the sediment at stations located along the Kaoping river and the north-western shelf of the Kaoping estuary. However, in the south-eastern shelf and some canyon sites, petroleum-derived PAHs were a more significant source of these compounds. Principal component analysis and hierarchical cluster analysis suggest PAHs in the sediments from the north-western shelf, and river and canyon sediments might be a pyrogenic product of coal and diesel-burning vehicles, while those of the south-eastern shelf may be petrogenic. PAH concentrations and compositional patterns are effective tracers of particulate transport in KPSC system. The seaward transport of riverine particulates was found to be mostly directed to NW-shelf and/or canyon.  相似文献   

7.
To assess the status of polycyclic aromatic hydrocarbon (PAH) contamination in coastal and riverine environments in Thailand, we collected 42 surface sediment samples from canals, a river, an estuary, and coastal areas in Thailand in 2003 and analyzed them for PAHs with 3-7 benzene rings by gas chromatography-mass spectrometry (GC-MS). The total concentration of PAHs ranged from 6 to 8399 ng/g dry weight. The average total PAH concentrations were 2290+/-2556 ng/g dry weight (n=8) in canals, 263+/-174 (n=11) in the river, 179+/-222 (n=9) in the estuary, and 50+/-56 (n=14) in coastal areas. Comparison of the concentration range with a worldwide survey of sedimentary PAH concentrations ranked PAH contamination in Thai sediments as low to moderate. The ratio of the sum of methylphenanthrenes to phenanthrene (MP/P ratio) allows discrimination of PAH sources between petrogenic (>2) and pyrogenic (<0.5) origins. Sediments from urban canals in Bangkok showed the highest PAH concentrations and petrogenic signatures (MP/P=1.84+/-0.98 [n=6] in canal sediments) with abundant alkylated PAHs, indicating major sources of petrogenic PAHs in the city. To identify the sources of the petrogenic inputs in Thailand, we analyzed triterpanes, biomarkers of petroleum pollution, in the sediment samples and in potential source materials. Hopane profiles were remarkably uniform throughout the nation, suggesting a diffuse single source (e.g. automobiles). Molecular profiles of hopanes and PAHs in sediments from the urban canals were similar to those in street dust, indicating that street dust is one of the major sources of petrogenic PAHs in the urban area. On the other hand, low levels of PAHs (approximately 50 ng/g) with a pyrogenic signature (MP/P ratio approximately 0.5) were widely recorded in remote areas of the coast and the Chao Phraya River. These pyrogenic PAHs may be atmospherically transported throughout the nation. Middle and lower reaches of the Chao Phraya River, the river mouth, and the upper Gulf of Thailand showed intermediate concentrations and profiles of PAHs, indicating mixtures of petrogenic and pyrogenic origins. Perylene was abundant in sediments, representing up to approximately 60% of total identified PAHs. High inputs of soil due to frequent heavy rains could contribute to the high perylene abundance in the sediments. Sedimentary PAH concentrations decreased offshore with a half distance of approximately 10 km in the upper Gulf off the mouth of the Chao Phraya River. This is probably due to active deposition of laterally transported riverborne particles.  相似文献   

8.
The fate of polycyclic aromatic hydrocarbon (PAH) contamination in a mangrove swamp (Yi O) in Hong Kong after an oil spill accident was investigated. The concentrations and profiles of PAHs in surface sediments collected from five quadrats (each of 10 m×10 m) covering different degrees of oil contamination and the most contaminated mangrove leaves were examined in December 2000 (30 days after the accident) and March 2001 (126 days later). The concentrations of total PAHs in surface sediments ranged from 138 to 2135 ng g−1, and PAHs concentrations decreased with time. In the most contaminated sediments, total PAHs dropped from 2135 (30 days) to 1196 ng g−1 (120 days), and the decrease was smaller in less contaminated sediments. The percentage reduction in sediment PAHs over three months (44%) was less significant than that in contaminated leaves (85%), indicating PAH in or on leaves disappeared more rapidly. The PAH profiles were very similar in sediments collected from quadrats Q1 and Q2 with benzo[a]anthracene and pyrene being the most abundant PAH compounds, but were different in the other three quadrats. The proportion of the light molecular weight PAHs to total PAHs increased after three months, especially phenanthrene. Results suggest that physical and photo-chemical weathering (tidal washing and photo-oxidation) of crude oil in surface sediments and on plant leaves were important processes in the first few months after the oil spill. The PAH contamination in Yi O swamp came from both petrogenic and pyrolytic sources. The petrogenic characteristic in the most contaminated sediment was confirmed with high values of phenanthrene to anthracene ratio (>10) and low values of fluoranthene to pyrene ratio (0.3–0.4).  相似文献   

9.
To assess the contamination of polycyclic aromatic hydrocarbons (PAHs) in the Mediterranean coastal environment of Egypt, 26 sediment samples from the coastline, harbours, estuaries and coastal lakes were collected and analyzed. The sediment PAH concentrations of thirty-nine 2-6 ring PAHs ranged from 13.5 to 22,600 ng/g. PAH profiles varied according to the nature of the site and its proximity to sources. Industrialized and urbanized region showed high level of PAHs contamination. In general, the contamination levels of PAHs were similar to those observed in contaminated and slightly contaminated sediments of the Mediterranean Sea. Molecular indices based on ratios of selected PAH concentrations were used to differentiate PAHs from pyrogenic and petrogenic and mixed origins. Good correlations were observed between the petrogenic index, MP/P, A-PAHs/P-PAHs and HMW/LMW. Finally, PAH levels in sediments were compared with Sediments Quality Guidelines (ERM-ERL) for evaluation of probable toxic effects on organism.  相似文献   

10.
We collected surface sediment samples from 174 locations in India, Indonesia, Malaysia, Thailand, Vietnam, Cambodia, Laos, and the Philippines and analyzed them for polycyclic aromatic hydrocarbons (PAHs) and hopanes. PAHs were widely distributed in the sediments, with comparatively higher concentrations in urban areas (∑PAHs: ∼1000 to ∼100 000 ng/g-dry) than in rural areas (∼10 to ∼100 g-dry), indicating large sources of PAHs in urban areas. To distinguish petrogenic and pyrogenic sources of PAHs, we calculated the ratios of alkyl PAHs to parent PAHs: methylphenanthrenes to phenanthrene (MP/P), methylpyrenes + methylfluoranthenes to pyrene + fluoranthene (MPy/Py), and methylchrysenes + methylbenz[a]anthracenes to chrysene + benz[a]anthracene (MC/C). Analysis of source materials (crude oil, automobile exhaust, and coal and wood combustion products) gave thresholds of MP/P = 0.4, MPy/Py = 0.5, and MC/C = 1.0 for exclusive combustion origin. All the combustion product samples had the ratios of alkyl PAHs to parent PAHs below these threshold values. Contributions of petrogenic and pyrogenic sources to the sedimentary PAHs were uneven among the homologs: the phenanthrene series had a greater petrogenic contribution, whereas the chrysene series had a greater pyrogenic contribution. All the Indian sediments showed a strong pyrogenic signature with MP/P ≈ 0.5, MPy/Py ≈ 0.1, and MC/C ≈ 0.2, together with depletion of hopanes indicating intensive inputs of combustion products of coal and/or wood, probably due to the heavy dependence on these fuels as sources of energy. In contrast, sedimentary PAHs from all other tropical Asian cities were abundant in alkylated PAHs with MP/P ≈ 1-4, MPy/Py ≈ 0.3-1, and MC/C ≈ 0.2-1.0, suggesting a ubiquitous input of petrogenic PAHs. Petrogenic contributions to PAH homologs varied among the countries: largest in Malaysia whereas inferior in Laos. The higher abundance of alkylated PAHs together with constant hopane profiles suggests widespread inputs of automobile-derived petrogenic PAHs to Asian waters.  相似文献   

11.
The spatial distribution of aliphatic and polycyclic aromatic hydrocarbons (PAHs) was investigated in sediments from the Cienfuegos bay. The highest anthropogenic hydrocarbon inputs were found near the city of Cienfuegos with an unresolved complex mixture (UCM) of aliphatic hydrocarbons and alkylated PAHs, indicative of petrogenic inputs. Parent PAHs, which are typical of high-temperature combustion processes, were evenly distributed in the whole basin and largely prevailing in the southern part of the Cienfuegos city. Biomarker fingerprints assign the sources of pollution to mixes of national and non-national crude oils. The overall levels of anthropogenic hydrocarbons are relatively high compared to relevant areas worldwide and reveal a moderate/high level of hydrocarbon pollution. The Cienfuegos bay sediments received over a period of 5 yr, 50 T/yr of petrogenic unresolved hydrocarbons (UCM) and 2 T/yr of PAHs, being deposited the 80% in the sediments of the north basin.  相似文献   

12.
The composition and distribution of aliphatic (n-alkanes) and polyaromatic hydrocarbons (PAHs) were measured for the surface sediments collected at 25 sites from Jiaozhou Bay, Qingdao, China. Total n-alkanes and PAH concentrations ranged from 0.5 to 8.2 microg/gdw and 0.02 to 2.2 microg/gdw, respectively, and the distribution of both n-alkanes and PAHs showed large spatial variations in the bay. The distribution of PAHs in the sediments was predominated by the three or more ring compounds. High hydrocarbon levels were generally found in the areas associated with high anthropogenic impact and port activities in the bay. The calculated hydrocarbon indexes suggest that petroleum contamination was the main source of n-alkanes, while both pyrolytic and petrogenic sources contributed PAHs to the surface sediments of Jiaozhou Bay. In comparison to other polluted coastal sediments, the level of contamination from both aliphatic hydrocarbons and PAHs in Jiaozhou Bay sediments is relatively low at the present time.  相似文献   

13.
Aliphatic and aromatic hydrocarbons in coastal Caspian Sea sediments   总被引：17，自引：0，他引：17  
This investigation represents the first extensive study of the spatial distribution and sources of aliphatic (n-alkanes and unresolved complex mixture of fossil hydrocarbons) and polycyclic aromatic hydrocarbons (PAHs) in coastal sediments from the Caspian Sea. PAH concentrations, n-alkanes and biomarker profiles all suggested that there was limited petrogenic contamination in the shallow North Caspian Sea sediments, which are coarse with a low total organic carbon content. In contrast, moderate to high petrogenic contamination was found in the South Caspian Sea, in particular in the offshore oil fields near Baku, Azerbaijan. Contaminant patterns indicated that the PAHs were mainly from fossil sources, with higher contributions of pyrolytic only near industrialized and urban areas. A high contribution of perylene, a geochemically derived PAH, to the total PAHs was found in the west and south at sites influenced by the Kura, Safid Rud, Terek, Sulak and Samur Rivers.  相似文献   

14.
This investigation showed that urban stormwater runoff provides a significant amount of petrogenic material to receiving waters and sediments. A characteristic hydrocarbon ‘fingerprint’ for sediments and particulate matter in the Hillsborough Reservoir, Hillsborough River and upper Hillsborough Bay was provided. Determination of source material for petroleum contamination in stormwater runoff and river sediment indicated that crankcase oil was a primary contributor to sediment hydrocarbon contamination. A comparison of sediment hydrocarbons with hydrocarbons from stormwater runoff showed that the most probable source of crankcase oil-like petrochemicals found in sediment was the stormwater runoff.A comparison of hydrocarbon composition in suspended particulate matter with that of accumulated bottom sediments in the reservoir, river and bay, during a non-storm period and rising tide showed no resuspension and upriver transport of petroleum contaminated bay sediment. No special influence of the bay upon the lower river was observed relative to hydrocarbon tracers, indicating that most contaminated sediment transport was downriver during storm events. Additional studies should be performed over various tidal cycles and storm events incorporating sediment cores, sediment grain size analysis and hydrocarbon characterization at more closely spaced stations near the river mouth to address adequately the question of specific hydrocarbon pollution sources, rate of petroleum influx and persistence of petrochemical contaminants in the sediment.  相似文献   

15.
Data on the concentration and composition of aliphatic and polyaromatic hydrocarbons in the surface layer and the body of bottom sediments in Volga delta and on the northern Caspian shelf are given. Volga delta sediments are shown to contain large concentrations of organic compounds. It is established that the concentrations of organic compounds is largely dependent on the dispersiveness of sediments. Anthropogenic hydrocarbons, both oil and pyrogenic, fail to pass the marginal filter of the Volga River and do not reach the open part of the sea. Therefore, the hydrocarbons contained in the bottom sediments on the Caspian Sea shelf are mostly of natural genesis. The distribution of organic compounds in the bottom sediment strata has a complex character. In some cases, their concentration increases because of the higher flux of hydrocarbons (especially, polyarenes in the 1950s).  相似文献   

16.
Contaminations in sediments by polycyclic aromatic hydrocarbons (PAHs) and alkylated PAHs were investigated at 44 sites in Osaka Bay, Japan. Concentrations of total PAHs and alkylated PAHs were in the range 6.40–7800 ng/g dry weights and 13.7–1700 ng/g dry weights, respectively. The PAH concentrations tended to be higher along the shoreline in the vicinities of big ports, industrialized areas, and densely populated regions such as the cities of Osaka and Kobe. The major sources appeared to be pyrogenic or both pyrogenic and petrogenic at most of the sites. PAH concentrations were remarkably high at a site near Kobe, where the concentrations of dibenzo(a,h)anthracene and benzo(g,h,i)perylene exceeded the effects-range-medium concentration and eight PAHs were above the corresponding effects-range-low concentrations. Those PAHs may have been derived from the great fire associated with the large earthquake in 1995.  相似文献   

17.
The nature, origin and distribution of US EPA polycyclic aromatic hydrocarbons (PAHs) in the sediments of Olbia harbor (North Sardinia, Italy) were investigated by gas-chromatography/mass spectrometry (GCMS). PAH concentrations in the sediments (SigmaPAHs) ranged from 0.16 to 0.77 microg g(-1), indicating a homogeneously low level of pollution. A rather exceptional prevalence of low molecular weight PAHs was substantiated: nearly 80% of SigmaPAHs include naphthalene (15.19%) and phenanthrene (64.47%). Carcinogenic compounds were present in very low (BaP, BkF, BaA and DBA) or negligible (BbF and Inp) concentrations. As indicated by the Phen/Ant molar ratio, the main source of PAHs is petrogenic, probably due to oil spills from shipping. The low/high molecular weight ratio (ranging between 1.2 and 26) distinguishes the sediments of the tourist harbor from those of the commercial/industrial harbor. Moreover, a slight but meaningful pyrolytic contribution to pollution was found in the tourist harbor, which has the most polluted sediments in the whole harbor. Finally, good linear correlations were found between a selected PAH (Phen and Naph) and selected sums of PAHs (i.e. the total amount of the other 15 US EPA and the sum of low molecular weight PAHs).  相似文献   

18.
Sedimentary hydrocarbons have been studied quantitatively and qualitatively in 11 coastal stations located in the Gulf of Fos (French Mediterranean coast). Hydrocarbon levels ranged from 10 to 260 mg kg(-1) sed. dry weight. A new parameter "NAR" (Natural n-alkane ratio) is proposed to evaluate the contribution of terrestrial inputs of hydrocarbons in the sediments. The origins of hydrocarbons are multiple: terrestrial inputs, biogenic, pyrolytic (industry emissions mainly steel and iron industries, ship and road traffic). Generally, the main source of contamination is not petroleum. Several ratios between parent polycyclic aromatic hydrocarbons show that the sources of hydrocarbons in the sediments are generally much more pyrolytic than petrogenic.  相似文献   

19.
《Marine pollution bulletin》2013,71(1-2):266-273
Polycyclic aromatic hydrocarbons (PAHs) and aliphatic hydrocarbons (AHs) have been quantified for surface sediments collected from the East China Sea (ECS). Our results showed that relatively high levels of PAHs and AHs occurred in both the inner and outer mud areas, while their concentrations at the control site were much lower. AHs for all samples were dominated by the unresolved complex mixture (UCM). Results from diagnostic ratios revealed that sedimentary PAHs were mainly originated from mixed combustion residues of biomass, coal, and petroleum. Combustion residues of petroleum and oil were responsible for the presence of high AHs concentrations. We also conducted factor analysis (FA) to further characterize the PAH and AH sources. Four factors were identified based on the loading of components and attributed to coal and wood combustion (Factor 1), traffic-related sources (Factor 2), petrogenic source (Factor 3) and natural gas combustion (Factor 4).  相似文献   

20.
Changes in the levels and spatial distribution of PAHs as a consequence of the Oder flood in the summer of 1997 were investigated in post‐flood sediments from the Oder River and the Oder Lagoon. The aim of this study was to identify sources of the PAH pollution and in particular investigate polluted sites (“hot spots”) in the most highly suspected locations of the drainage area. Molecular indices based on isomeric PAH ratios and the ratio of the parent PAHs to methylated PAHs were used to distinguish between the pollution sources. Elevated levels of PAHs were discovered in the post‐flood sediments of the Oder River in comparison to the average regional values. Elevated concentrations of PAHs were also found in fluffy layer samples taken from the Oder Lagoon and the Pomeranian Bight in late August. The highest concentrations of PAHs were observed near power plants or roads with heavy traffic. Most of the contamination originates from high temperature pyrogenic sources with some slight overlays of petrogenic sources. These increased concentrations of pyrogenic origin may be attributable to flooding of municipal and industrial waste disposal areas in the Oder River drainage.  相似文献   

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