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1.
Polycyclic aromatic hydrocarbons (PAH) and their alkyl homologs are distributed in sediments throughout the world. The qualitative PAH pattern is remarkably constant for most of the locations studied, and the quantitative PAH abundance increases with proximity to urban centers. These findings are consistent with anthropogenic combustion's being the major source of these compounds. Two non-combustion sources of PAH have also been noted: retene coming from abietic acid and perylene probably coming from various extended quinone pigments.  相似文献   

2.
Polycyclic aromatic (PAH) and aliphatic hydrocarbon compositions, organic carbon, nitrogen and lignin contents were determined in whole, unfractionated sediment from the Washington continental shelf and in discrete sediment fractions separated by particle size and density. At least 20 to 25% of perylene and PAH derived from pyrolytic processes and 50% of the retene measured in whole sediment are contained within organic C- and lignin-rich panicles of density ≤ 1.9 g/cc. These particles, which include primarily vascular plant remains and bits of charcoal, comprise less than 1% of the total sediment weight. In contrast, a series of methylated phenanthrene homologs, possibly of fossil origin, are concentrated in some component of the more dense, lithic matrix of the sediment. Equilibrium models of PAH sorption/desorption from aqueous phase onto small particles of high surface area do not appear applicable to the behavior of the major PAH types identified in this aquatic environment.  相似文献   

3.
New insights into the origin of perylene in geological samples   总被引：1，自引：0，他引：1  
The origin of the polycyclic aromatic hydrocarbon (PAH) perylene in sediments and petroleum has been a matter of continued debate. Reported to occur in Phanerozoic organic matter (OM), fossil crinoids and tropical termite mounds, its mechanism of formation remains unclear. While a combustion source can be excluded, structural similarities to perylene quinone-like components present in e.g. fungi, plants, crinoids and insects, potentially suggest a product-precursor relationship. Here, we report perylene concentrations, 13C/12C, and D/H ratios from a Holocene sediment profile from the Qingpu trench, Yangtze Delta region, China. Perylene concentrations differ from those of pyrogenic PAHs, and rise to prominence in a stratigraphic interval that was dominated by woody vegetation as determined by palynology including fungal spores. In this zone, perylene concentrations exhibit an inverse relationship to the lignin marker guaiacol, D/H ratios between −284‰ and −317‰, similar to the methoxy groups in lignin, as well as co-variation with spores from wood-degrading fungi. 13C/12C of perylene differs from that of land plant wax alkanes and falls in the fractionation range expected for saprophytic fungi that utilise lignin, which is isotopically lighter than cellulose and whole wood. During progressive lignin degradation, the relative carbon isotopic ratio of the perylene decreases. We therefore hypothesise a relationship of perylene to the activity of wood-degrading fungi. To support our hypothesis, we analysed a wide range of Phanerozoic sediments and oils, and found perylene to generally be present in subordinate amounts before the evolutionary rise of vascular plants, and to be generally absent from marine-sourced oils, few exceptions being attributed perhaps to a contribution of marine and/or terrestrial-derived fungi, anoxia (especially under marine conditions) and/or contamination of core material by fungi. A series of low-molecular-weight aromatic quinones bearing the perylene-backbone were detected in Devonian and Cretaceous sediments, potentially representing precursor components to perylene.  相似文献   

4.
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5.
The past several decades have witnessed a significant expansion of mining activities in the Athabasca oil sands region, raising concerns about their impact on the surrounding boreal forest ecosystem. To better understand the extent to which distal sites are impacted by oil sands-derived airborne contaminants, we examine sources of polycyclic aromatic hydrocarbons (PAHs) in surface sediments and dated sediment cores from Saskatchewan lakes situated ∼100–220 km east–northeast of the main area of bitumen mining activities. The concentrations and fluxes of both parent and alkylated PAHs are low and show considerable variability over the past 70–100 years. Small yet discernible increases in PAH concentrations and fluxes occurred over the past 30 years, a trend which coincides with the rapid growth in bitumen production. However, several lines of evidence point to wildfires as the principal source of PAHs to these lakes: (1) the significant co-variations in most cores between retene (1-methyl-7-isopropyl phenanthrene) and other groups of parent and alkylated PAHs, (2) the similarity in compound specific δ13C signatures of the parent PAHs phenanthrene and pyrene in recently deposited surficial sediments and those corresponding to time intervals considerably pre-dating the large scale development of the oil sands and (3) the discernible up-core increases in the proportion of refractory carbon (i.e., char) in Rock-Eval 6 data. The collective evidence points to softwood combustion from boreal forest fires as the principal source of retene in sediments and the general increase in forest fire activity in this region over the past several decades as the source of refractory carbon. Mining activities associated with the Athabasca oil sands are thus not considered a major source of PAHs to these lakes.  相似文献   

6.
Polycyclic aromatic hydrocarbon (PAH) compositions were determined in plankton, sediment-trap-collected particulate material and sediment cores from Dabob Bay using a high performance liquid Chromatographie (HPLC)/fluorescence technique. The annual flux of individual PAH measured in a series of sediment traps was compared with the flux of corresponding compounds determined from 210Pb dated bottom sediments. Systematic seasonal variations in the fluxes and concentrations of PAH, Al and organic carbon in the trap-collected particulates and seasonally collected plankton were also investigated to determine whether or not PAH are associated with either terrestrial or marine-derived materials.Concentrations of all PAH studied increased tenfold within the last 80–100 yr of sediment deposition, except for perylene which displayed a reasonably constant concentration profile. This suggests at least two sources contribute to the observed sedimentary PAH compositions in Dabob Bay, i.e., anthropogenic combustion and a natural source. Plankton and sediment trap-collected particulates contained PAH mixtures qualitatively similar to underlying surface sediments. Microscopic examination indicated fecal pellets were the major form of particulate material in the sediment traps. The fecal pellets collected in the sediment trap time series quantitatively account for essentially 100% of the PAH fluxes measured in the 210Pb dated sediments, implying Zooplankton fecal pellets control the removal of PAH to Dabob Bay sediments. These measurements provide clear evidence that the PAH studied are not produced after sediment deposition. The observed seasonal covariations of PAH and Al in both sediment trap and plankton samples further indicate that PAH originate from terrestrially-based sources, are introduced into the marine environment by runoff and erosion or atmospheric deposition and are not produced by marine plankton.  相似文献   

7.
Perylene and penta-aromatic hydrocarbons were determined in sediments as part of a study that was dedicated to the aquatic ecosystem of Elelenwo Creek (Southern Nigeria) in order to carry out a critical corroboration of occurrence and diagenetic evolution of perylene in the sediments of the creek. The results show that the annual mean levels of Benzo [g, h, i] Perylene ranged from 209.00–245.28 ?g/kg dry weight at the various stations sampled. Meanwhile, Station 3 recorded the highest mean level of 245.28 ?g/kg dry weight. The observed values for total penta-aromatic hydrocarbons were high (787.00–1154.36?g/kg dry weight) in all the stations sampled. In addition, the highest mean value of 1154.36?g/kg dry weight was again recorded at station 3 for the penta-aromatic hydrocarbons. One origin index or concentration ratio of Ip/Ip+BghiP was also used to evaluate the suitability of the penta-aromatic hydrocarbons as a tracer to distinguish between contaminations arising from different sources. The values for the sampling stations therefore ranged from 0.41 to 0.43. A critical appraisal of the PAH index, consequently, suggested that petroleum combustion is the major penta-aromatic hydrocarbon source in sediments of the creek. The PAH group profile shows that perylene was high in the sediments and would pose apparent effects in fauna. The high concentration of perylene in the sediments was also indicative of an in situ biogenic derivation. Furthermore, a concentration of perylene > 10 % of total penta-aromatic hydrocarbons established a credible diagenetic origin.  相似文献   

8.
The origin of perylene, a five-ring polycyclic aromatic hydrocarbon (PAH), in sediments has been a matter of constant debate and its formation mechanisms remain unclear. A perylene record in sediment was described and could support a clear link between perylene and terrigenous organic matter (OM) input. The distributions of PAHs, the variations of organic proxies such as the ratio of terrigenous to aquatic n-alkanes (TAR(HC)) and 5α(H)-stanols/Δ5-sterols ratio in sediments have been investigated. Sediments were sampled from a pond artificially created during the Middle Ages from a swampy area. In the period prior to the pond creation, for which high contributions of terrigenous OM were evidenced, perylene was found to be the predominant PAH. Furthermore, perylene content was shown to increase in response to the establishment of more reducing conditions. This result supports the common idea that the main source of perylene is natural and derives from biogenic precursors under reducing conditions. The creation of the pond in this wetland is marked by the deposition of a wood rich level characterized both by more oxygenated conditions and higher concentrations of perylene. These high concentrations could result from the introduction of high concentrations of biogenic precursors of perylene under oxidative conditions. Subsequently, the progressive burial of the woody level could have allowed the establishment of oxygen depleted conditions and the formation of perylene. These results validate the use of perylene as a paleoenvironmental marker of terrigenous sources but it must be carefully used as a marker for syn- or post-depositional oxygen depleted conditions in lacustrine environments.  相似文献   

9.
Sediment cores from Sagamore Lake and Woods Lake in New York State's Adirondack Park, an area remote from industrial activities, were analyzed for polynuclear aromatic hydrocarbons (PAH) by high resolution gas chromatography/mass spectrometry (GC/MS). Their composition and distribution with depth in the sediment indicate that the parental PAH in the surface sediments are primarily produced by anthropogenic combustion of fossil fuels. Perylene in deep sediments is apparently transformed from natural precursors in the reducing environment, however, the exact precursors remain unknown. The rather even sediment distributions of the non-parental PAH differ from the parental, suggesting biogenic origins. Based on their chemical structures, retene and alkylated and partially hydrogenated phenanthrenes are believed to be biogenically converted from abietic acid; hydrochrysenes and hydropicenes, from pentacyclic triterpenes.  相似文献   

10.
Sediment cores from two locations in Green Bay and two in lake Michigan were analyzed for 12 polycyclic aromatic hydrocarbons (PAHs), loss-on-ignition (LOI),210Pb,137Cs, and7Be to study differences in deposition patterns between the freshwater estuary Green Bay, with several local sources, and the open Lake Michigan, dominated by atmospheric inputs. We found that the remote sites receive relatively less high-molecular weight PAHs such as ideno(1,2,3-cd)pyrene and dibenz(ah)anthracene and are more depleted in anthracene and pyrene. This may be related to a low Henry’s law constant for the high molecular compounds and to selective photo-oxidation of anthracene and pyrene during transport. While sedimentation rates are higher in Green Bay than in the open lake, the PAH levels are generally comparable (0.3–8.5 μg g?1) in the two areas. However, the highest PAH levels are found in a core from Green Bay (GB88G). The two Green Bay cores have total PAH concentration maxima in 1985, which appear to be related to the combustion of petroleum. Also, one Green Bay core (GB88G) and the two from Lake Michigan exhibit PAH maxima in the early 1950s in agreement with observations from other study areas. There is a significant correlation between total PAH and LOI, and thus total organic carbon, for the Green Bay cores, but little or no such correlation for the Lake Michigan cores. This may indicate that PAHs in Green Bay are effectively scavenged by settling detritus.  相似文献   

11.
Four anoxic sediment cores were collected from Chini Lake, Malaysia in order to investigate the variability of polycyclic aromatic hydrocarbon (PAH) and perylene concentrations. The study also determined significant differences of perylene concentrations in different sediment layers. Total PAH concentrations ranged from 248 to 8098 ng g−1 in the samples. Diagnostic PAH ratios such as methylphenanthrenes/phenanthrene (MP/P), phenanthrene/anthracene (P/A) and fluoranthene/(fluoranthene + pyrene) (Fl/(Fl + Py) revealed a dominance of pyrogenic influences and partial petrogenic inputs to the top sediment layers. Perylene concentrations were high in the top layers (<12 cm) and increased with increasing depth. There is a significant positive correlation (r = 0.705, p = 0.01) between perylene concentrations and TOC. Analysis of variance (ANOVA) and LSD revealed significant differences (p < 0.05) in TOC-normalized perylene concentrations between the upper (<12 cm) and bottom layers (>12 cm). The average perylene concentrations accounted for 26–50% (0–12 cm) and 50–77% (12–36 cm) of pentacyclic-aromatic hydrocarbon isomers (PAI) present whereas it made up 10–34% (0–12 cm) and 46–66% (12–36 cm) of the total PAH. The average pyrene concentrations decreased with increasing depth and accounted for 62% (0–3 cm), 20–23% (3–12 cm) and 3–1.4% (12–36 cm) of perylene present. The results of hierarchical cluster analysis based on these ratios suggested different input sources for the top and bottom layers. It is concluded that the activity of termites on woody plants produced perylene which is supplied to the lake by run-off from the heavy and frequent rains in this Asian tropical climate. In addition, there was also in situ formation of perylene in the bottom layers due to diagenetic processes.  相似文献   

12.
Concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) were investigated in surface sediments of the Yellow River Estuary (YRE). The isobath-parallel tidal and residual currents play important roles in the variation of PAH distribution, such that the contamination level of PAHs in fine-grained sediments is significantly higher than in the relatively coarse grain size sediments. Both diagnostic ratios and principal component analysis (PCA) with multivariate linear regression (MLR) were used to apportion sources of PAHs. The results revealed that pyrogenic sources are important sources of PAHs. Further analysis indicated that the contributions of coal combustion, traffic-related pollution and mixed sources (spills of oil products and vegetation combustion) were 35, 29 and 36 %, respectively, using PCA/MLR. Pyrogenic sources (coal combustion and traffic-related pollution) contribute 64 % of anthropogenic PAHs in sediments, which indicates that energy consumption could be a predominant factor in PAH pollution of YRE. Acenaphthylene and acenaphthene are the two main species of PAHs with more ecotoxicological concern in YRE.  相似文献   

13.
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14.
Concentration, distribution, and sources of 16 polycyclic aromatic hydrocarbons (PAHs) were investigated in surface sediments of Laizhou Bay, China. Total PAH concentrations ranged from 97.2 to 204.8 ng/g, with a mean of 148.4 ng/g. High concentrations of PAHs were found in the fine-grained sediments on both sides of the Yellow River estuary (YRE). In contrast, low levels of PAHs were observed in relatively coarse grain sediments, suggesting hydrodynamics influence the accumulation of sedimentary PAHs. The YRE and its adjacent area is the main sink for Yellow River-derived PAHs. Both PAH isomer ratios and principal component analysis (PCA) with multivariate linear regression (MLR) were applied to apportion sources of PAHs. Results indicated that both pyrogenic and petrogenic PAH sources were important. Further PCA/MLR analysis showed that the contributions of coal combustion, petroleum combustion and a combined source of spilled oil and biomass burning were 41, 15 and 44%, respectively. From an ecotoxicological viewpoint, the studied area appears to have low levels of PAH pollution.  相似文献   

15.
Concentrations, spatial distribution and sources of 16 polycyclic aromatic hydrocarbons (PAHs) listed by the United States Environmental Protection Agency as priority pollutants were investigated in surface sediments of Bohai Bay, North China. Total concentrations of PAHs were in the range of 140.6–300.7 ng/g (dry wt), with an average of 188.0 ng/g. The three predominant PAHs were phenanthrene, acenaphthene and naphthalene. Sedimentary PAH concentrations of the north and central Bohai Bay were higher than those of the southern side of this bay. PAHs source analysis suggested that PAHs in most of the sediments were mainly from grass, wood and coal incomplete combustion. At other stations near the estuaries (Luanhe River Estuary and Chaohe River Estuary) or the oil drilling platform, both petrogenic and pyrogenic inputs were significant. The pyrogenic PAHs close to the oil drilling platform were mainly from petroleum combustion.  相似文献   

16.
Origin of perylene in ancient sediments and its geological significance   总被引：2，自引：0，他引：2  
The distributions of polycyclic aromatic hydrocarbons (PAHs) in sediments of three Upper Triassic to Middle Jurassic sedimentary sequences from the Northern Carnarvon Basin, Australia have been investigated. Perylene was found to be a major PAH component in the top Lower to base Middle Jurassic sediments that are immature or at low maturity. Its depth/age profiles are not related to the combustion-derived PAHs that have been believed to be produced during ancient vegetation fires before deposition. This suggests a diagenetic origin for perylene. The concentration of perylene in the sediments is proportional to the amount of terrestrial input, decreasing with distance from the source of land sediments. Its carbon isotope composition is slightly heavier than higher-plant derived PAHs, but still in the range of the terrestrially sourced PAHs including higher-plant PAHs and combustion-derived PAHs as suggested previously. Fungi are proposed to be the major precursor carriers for perylene in sediments based on the facts that (1) perylenequinone structures have been previously suggested to be the natural precursors for perylene; (2) perylenequinone pigments exist in many fungal bodies; (3) fungi have played an important role during geological processes.  相似文献   

17.
通过对祁连山冻土区天然气水合物DK-9孔不同深度岩心顶空气中的烃类气体组分及甲烷、乙烷的C同位素分析测试,对比分析了岩心顶空气组分含量变化与天然气水合物及其异常层段、油气显示层段、断层或破碎带分布之间的空间关系,探讨了顶空气组分对天然气水合物及其异常现象、油气显示现象、烃类气体运移作用及顶空气同位素对气体成因的指示意义。结果显示,岩心顶空气中烃类气体含量高的深度段180.26~308.50m、356.45~399.32m、458.55~508.65m与天然气水合物及其异常层段、油气显示层段具有较好的对应关系,其高值区间可作为天然气水合物、油气显示的一种指示。距断层或破碎带产出位置不同的岩心顶空气组分含量变化显示,不同级次的断裂系统为烃类气体向上运移提供了通道,部分可为天然气水合物提供一定的赋存空间;甲烷、乙烷C同位素数据显示气体以热解成因为主,部分为混合成因。  相似文献   

18.
Black carbon (BC) in soils plays a key role of carrying hydrophobic pollutants like polycyclic aromatic hydrocarbons (PAHs). However, little is known about the spatial distribution, sources of BC and its relationship with PAHs in urban soils. We studied BC, total organic carbon (TOC) and PAHs concurrently in 77 soils collected from downtown area, suburban and rural area and industrial area of Shanghai, China. BC was determined by both chemical oxidation (dichromate oxidation, BCCr) and chemo-thermal oxidation (CTO-375, BCCTO). BC sources were identified qualitatively by BC/TOC concentration ratios and BC-cogenerated high molecular weight (HMW) PAH isomer ratios and quantitatively by principal component analysis followed by multiple linear regression (PCA-MLR). Results showed that BCCr concentration (4.65 g/kg on average) was significantly higher than BCCTO (1.91 g/kg on average) in Shanghai soils. BCCr concentrations in industrial area were significantly higher than those in other two. Stronger correlation was found between PAHs and TOC, BCCr than that between PAHs and BCCTO, which indicates the possibility of PAHs being carried by charcoal and other organic matters thus negating its exclusive dependence on soot. Charcoal was therefore suggested to be taken into account in studies of BC and its sorption of PAHs. BC/TOC ratios showed a mixed source of biomass burning and fossil fuel combustion. PCA scores of BC-cogenerated HMW PAHs isomer ratios in potential sources and soil samples clearly demonstrated that sources of BC in urban soils may fall into two categories: coal and biomass combustion, and traffic (oil combustion and tire wear). PCA-MLR of HMW PAHs concentrations in soil samples indicated that coal and oil combustion had the largest contribution to BC in urban soils while tire wear and biomass combustion were important in downtown and rural area, respectively, which indicated they were main sources of HMW PAHs and presumably of BC.  相似文献   

19.
The burial characteristics and toxicity risks associated with n-alkanes and polycyclic aromatic hydrocarbons (PAHs) in the riverine and estuarine sediments of the Daliao River watershed were investigated based on three sediment cores. The sum of the n-alkane and PAH concentrations, normalized to organic carbon (OC), ranged from 0.27 to 63.09 μg g?1OC?1 and 6.60 to 366.20 μg g?1OC?1, respectively. The features and the history of industrial activities, such as the oil and chemical industries and port activities near the river and estuary, resulted in different distributions and sources of hydrocarbons. The sources of pollution were identified based on n-alkane indexes and on diagnostic ratios of PAHs. The diagnostic ratios indicated that the n-alkanes were derived from both biogenic and petrogenic sources in different proportions and that the PAHs were derived primarily from petrogenic combustion sources. A hierarchical cluster analysis grouped the core samples into two clusters. The first cluster, river sediments, corresponded to industrial activities; the second cluster, estuarine sediments, corresponded to port shipping activities. The toxic potency of the PAHs in the cores was assessed in terms of toxic equivalents (TEQs) of dibenzo[a,h]anthracene and benzo[a]pyrene. The top layer of the sediment in the cores had a relatively high toxicity. The TEQ values for benzo(a)pyrene (TEQBaP) and dioxins (TEQTCDD) furnished a consistent assessment of the PAHs in the sediment cores.  相似文献   

20.
《Applied Geochemistry》2001,16(11-12):1429-1445
Polycyclic aromatic hydrocarbons (PAHs) were measured in surface sediments and dated core sediments from the Pearl river and estuary, China, to investigate the spatial and temporal variability of anthropogenic pollutants. The sediments from the sampling stations at the Guangzhou channel have the highest concentrations of PAHs, owing to contributions from the large amount of urban/industrial discharges from the city of Guangzhou. The significant decrease of PAHs concentrations in sediments from the Shiziyang channel is mainly attributed to the increasing degradation and desorption of low molecular weight PAHs and alkyl PAHs, and the dilution by less contaminated water and particles from the East river. The PAH contaminants were concentrated on the western side in the Lingding bay of the Pearl river estuary because of the hydrodynamic and sedimentation conditions. Based on the characteristics of the parent compound distributions (PCDs) and the alkyl homologue distributions (AHDs) of PAHs, the potential source of PAHs in sediments from each sampling station was identified. Results indicated that the pyrogenic (combustion) source, characterized by the abundance of parent PAHs, were predominant in the heavily contaminated station (ZB01) near the aging industrial area, and the petrogenic (petroleum- derived) PAHs were more abundant in the stations (ZB02, ZB03) adjacent to the petrochemical plant and shipping harbor. Sediments from Lingding bay show variable distributions of PAH composition and variety in the proportion of combustion and petrogenic sources for the PAHs in different stations. Perylene, a naturally derived PAH, was found to be highly abundant in less contaminated stations. Analysis of the dated sediments (210Pb) indicates that higher PAH concentrations occurred in the sediments deposited after 1980, and higher fluxes of PAHs discharged to the Pearl river are found after 1990.  相似文献   

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