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1.
Valleys tributary to the Mississippi River contain fossiliferous slackwater lake sediment (Equality Formation) deposited in response to aggradation of the Mississippi River valley during the last glaciation. In the St. Louis Metro East area, the lower part of the Equality Formation is primarily laminated, fossiliferous silt and clay deposited from about 44,150 to 24,310 14C yr B.P. The upper Equality Formation is primarily very fine sand to silt deposited from about 21,200 to 17,000 14C yr B.P. Among the four cores that sample this succession in the St. Louis Metro East area, core MNK-3 (38.64EN, 90.01EW) was selected for detailed study. Three sources are distinguished by the following characteristics: (1) gray smectite-quartz-Se-rich, feldspar-poor material of the Des Moines, Wadena, and James lobes; (2) reddish brown kaolinite-Cu-Fe-rich sediment of the Superior and Rainy lobes; and (3) brown illite-dolomite-Sr-rich sediment of the Lake Michigan and Green Bay lobes. The earliest sediments (44,150 to 41,700 14C yr B.P.) were derived from the central and western provenances and are chronocorrelative with the lower Roxana Silt. A hiatus occurred from about 41,700 to 29,030 14C yr B.P. when much of the middle Roxana Silt (Meadow Member) was deposited on adjacent uplands. The youngest sediment includes evidence of heightened activity of the Superior Lobe at about 29,000 14C yr B.P., the Lake Michigan and Green Bay lobes from about 25,000 to 24,000 14C yr B.P., and the Wadena-Des Moines-James lobes at about 21,000 14C yr B.P.  相似文献   

2.
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   

3.
Understanding the natural mechanisms that control fire occurrence in terrigenous ecosystems requires long and continuous records of past fires. Proxies, such as sedimentary charcoal and tree-ring fire scars, have temporal or spatial limitations and do not directly detect fire intensity. We show in this study that polycyclic aromatic hydrocarbons (PAHs) produced during wildfires record local fire events and fire intensity. We demonstrate that high performance liquid chromatography with fluorescence detector (HPLC-FLD) is superior to gas chromatography–mass spectrometry (GC–MS) for detecting the low concentrations of sedimentary PAHs derived from natural fires. The HPLC-FLD is at least twice as sensitive as the GC–MS in selective ion monitoring (SIM) mode for parent PAHs and five times as sensitive for retene. The annual samples extracted from varved sediments from Swamp Lake in Yosemite National Park, California are compared with the observational fire history record and show that PAH fluxes record fires within 0.5 km of the lake. The low molecular weight (LMW) PAHs (e.g., fluoranthene, pyrene and benz[a]anthracene) are the best recorders of fire, whereas the high molecular weight (HMW) PAHs likely record fire intensity. PAHs appear to resolve some of the issues inherent to other fire proxies, such as secondary deposition of charcoal. This study advances our understanding of how PAHs can be used as markers for fire events and poses new questions regarding the distribution of these compounds in the environment.  相似文献   

4.
Oyster and sediment samples collected from six sites in Galveston Bay from 1986 to 1998 were analyzed for polynuclear aromatic hydrocarbons (PAHs). Total concentrations of parent PAHs in oysters ranged from 20 ng g−1 at one site to 9,242 ng g−1 at another and varied randomly with no clear trend over the 13 year period at any site. Concentrations of alkylated PAHs, which are indications of petroleum contamination, varied from 20 to 80,000 ng g−1 in oysters and were in higher abundance than the parent PAHs, indicating that one source of the PAH contaminants in Galveston Bay was petroleum and petroleum products. Four to six ring parent PAHs, which are indicative of combustion source , were higher than those of 2–3 ring parent PAHs, suggesting incomplete combustion generated PAHs was another source of PAHs into Galveston Bay. Concentrations of parent PAHs in sediments ranged from 57 to 670 ng g−1 and were much lower than those in oysters. Sediments from one site had a high PAH concentration of 5,800 ng g−1. Comparison of the compositions and concentrations of PAHs between sediment and oysters suggests that oysters preferentially bioaccumulate four to six ring PAHs. PAH composition in sediments suggests that the sources of PAH pollution in Galveston Bay were predominantly pyrogenic, while petroleum related PAHs were secondary contributions into the Bay.  相似文献   

5.
Polycyclic aromatic hydrocarbons in the soils of technogenic landscapes   总被引：1，自引：0，他引：1  
An integrated study of qualitative and quantitative composition of polycyclic aromatic hydrocarbons (PAH) in the atmospheric precipitation-soil-lysimetric water system of aerotechnogenic polluted landscapes was conducted using high-performance liquid chromatography in a gradient mode. Only low-molecular weight polyarenes (phenanthrene, anthracene, fluoranthene, pyrene, benz(a)anthracene, and chrysene) were found in the atmospheric precipitation and lysimetric waters. The growth of PAHs in soils is provided by the input of phenanthrene, fluoranthene, and pyrene with atmospheric precipitation. The absence of heavy PAHs (benzfluoranthenes, benz(a)pyrene, dibenz(a,h)anthracene, benz(ghi) perylene, and indeno[1,2,3-cd]pyrene) in the atmospheric precipitation and their identification in soil give grounds to state that their accumulation was caused mainly by transformation of organic matter during pedogenesis. The technogenic impact was estimated and criterion of the degree of soil pollution by PAH was proposed.  相似文献   

6.
《Organic Geochemistry》1999,30(8):937-945
The anaerobic degradation of the polycyclic aromatic hydrocarbons (PAHs) naphthalene and phenanthrene was investigated in several marine harbor sediments. In sediments from Boston Harbor that were heavily contaminated with petroleum, [14C]-naphthalene and [14C]-phenanthrene were oxidized to 14CO2 without a lag, suggesting that the microbial community was adapted for anaerobic PAH oxidation in situ. The addition of molybdate, a specific inhibitor of sulfate-reducing microorganisms, inhibited PAH mineralization which suggested that sulfate reducers were involved in the anaerobic oxidation of the PAHs. PAHs were also anaerobically oxidized at another site in Boston Harbor that was less heavily contaminated, but at a slower rate than in the most heavily contaminated sediments. Sediments not contaminated with petroleum did not significantly oxidize the PAHs. A similar correspondence between rates of anaerobic PAH oxidation and the degree of PAH contamination was observed in sediments from Tampa Bay and San Diego Bay. When relatively pristine sediments from San Diego Bay that did not have a significant capacity for anaerobic PAH oxidation were exposed to high concentrations of naphthalene, they developed a potential for naphthalene degradation that was comparable to that in sediments that had a history of PAH contamination. The increase in potential for naphthalene degradation in the sediments exposed to naphthalene was associated with an increase in naphthalene-degrading microorganisms. These results suggest that many marine harbor sediments contain microorganisms capable of anaerobically oxidizing PAHs under sulfate-reducing conditions and that these microorganisms will respond with an increase in their activity when PAHs are introduced into the sediments. Thus, if PAH inputs into harbor sediments from petroleum can be reduced there may be a widespread potential for microorganisms to remove this PAH contamination from the sediments, despite anaerobic conditions.  相似文献   

7.
The present work is the first attempt to compare the data of a comprehensive study of the origin and distribution of 16 priority pollutant polycyclic aromatic hydrocarbons (PAHs) in surface sediments (<63 μm) from 18 sampling stations, 9 from Sundarban of Bangladesh and 9 from Indian counterpart. Σ19PAHs concentration in sediments showed wide variations from 208.3 to 12,993.1 ng g?1 dry weight in Indian Sundarban, whereas 208.4 to 4,687.9 ng g?1 in the case of Bangladesh. Fluoranthene, pyrene, benzo(b)fluoranthene, benzo(a)pyrene and dibenzo(a,h)anthracene were predominant species for both the countries. The PAH diagnostic ratios indicated that the PAHs in sediments from both the countries were of mixed source of hydrocarbons of both petrogenic and pyrolytic origin. According to the numerical effect-based sediment quality guidelines, the levels of PAHs in the Sundarban wetland of Bangladesh and India should not exert adverse biological effects. The TEQ values calculated for samples from the Bangladesh and Indian Sundarban varied from 13.68 to 1,014.75 and 1.31 to 2,451 ng g?1 d.w. with an average of 221.02 and 358.63 ng g?1, respectively. The overall contamination status of PAH was higher in India than Bangladesh.  相似文献   

8.
孔祥胜  苗迎 《地球学报》2014,35(2):239-247
为证实大气干湿沉降物是岩溶地下河中多环芳烃(PAHs)的来源,研究选择了某城市典型的岩溶地下河水源地作为研究地点,采用大气干湿采样器、聚氨酯泡沫(PUF)大气被动采样器分别采集大气及其干湿沉降物样品,同时采集地下河水样和分层采集流域土壤,利用气相色谱-质谱联用仪(GC-MS)测定了16种PAHs优先控制污染物。结果表明,地下河流域大气干湿沉降中PAHs的干湿沉降通量为147.26 ng·(m2·d)-1,流域PAHs沉降量为1943.8 g;大气中的PAHs浓度为45.33 ng·m-3;地下河水中PAHs浓度平均值为220.98 ng·L-1;土壤中PAHs浓度为38.72 ng·g-1;大气、降雨和土壤中PAHs组成以2~3环的萘、芴、菲、荧蒽、芘5种为主,地下河水中以芴、菲、荧蒽、芘、苯并[a]蒽、苯并[a]芘6种为主。利用地下河多介质中的16种PAHs成分谱、特征比值结合它们的物理化学性质进行PAHs的源解析,研究显示大气干湿沉降是岩溶地下河水中多环芳烃的主要污染源之一,这归因于岩溶地区防污性能的脆弱性。  相似文献   

9.
To examine the role of physical disturbance on the long-term preservation of polycyclic aromatic hydrocarbons (PAHs) in sediments, cores were collected from two sites removed from point sources of PAHs and representing contrasting seabed mixing regimes. Although ΣPAH concentrations in sediments over the past 50 years were not significantly different between the two sites, several PAH isomer ratios were significantly different (P<0.05) between the two sites. Downcore changes in PAH isomer ratios resulted from preferential losses of the more linear PAH isomers. Thus, episodic, intense seabed mixing contributes to more efficient removal of selected PAHs. However, PAHs are still sufficiently stable relative to mixing events that historical PAH profiles can be used to reconstruct major resuspension events.  相似文献   

10.
This study evaluates the accuracy of optically stimulated luminescence to date well-preserved strandline sequences at Manistique/Thompson bay (Lake Michigan), and Tahquamenon and Grand Traverse Bays (Lake Superior) that span the past ∼4500 yr. The single aliquot regeneration (SAR) method is applied to produce absolute ages for littoral and eolian sediments. SAR ages are compared against AMS and conventional 14C ages on swale organics. Modern littoral and eolian sediments yield SAR ages <100 yr indicating near, if not complete, solar resetting of luminescence prior to deposition. Beach ridges that yield SAR ages <2000 yr show general agreement with corresponding 14C ages on swale organics. Significant variability in 14C ages >2000 cal yr B.P. complicates comparison to SAR ages at all sites. However, a SAR age of 4280 ± 390 yr (UIC913) on ridge77 at Tahquamenon Bay is consistent with regional regression from the high lake level of the Nipissing II phase ca. 4500 cal yr B.P. SAR ages indicate a decrease in ridge formation rate after ∼1500 yr ago, likely reflecting separation of Lake Superior from lakes Huron and Michigan. This study shows that SAR is a credible alternative to 14C methods for dating littoral and eolian landforms in Great Lakes and other coastal strandplains where 14C methods prove problematic.  相似文献   

11.
Abundance, sources, and historical records of polycyclic aromatic hydrocarbons (PAHs) in sediment cores of three lakes located in northeast China were evaluated. One lake was located in a rural oil field area, one in an industrial urban oil field area, and the third in an urban industrialized area without oil field influence. Cores from each lake were divided into 1-cm sections, dated using 137Cs techniques, and 16 priority PAH compounds were measured. Total PAH concentrations were greater in industrial areas than in rural area, regardless of associated oil production. Only petroleum sources of PAHs were identified in lakes near oil fields between 1950s and 1980s, while sources of liquid fossil fuel combustion were persistently identified in the industrial urban lake. From 1990s to 2000s, PAH concentrations, especially high molecular weight PAHs, significantly increased in all lakes, which were consistent with the economic development in China, suggesting a change in energy use from wood burning and petroleum (oil) to liquid fossil fuel combustion. Environmental risk was low to moderate in sediments of the three lakes studied, and increases in high molecular weight PAHs during 1900s–2000s is a concern.  相似文献   

12.
Attention has been paid for the levels, sources and health risks of atmospheric aliphatic and polycyclic aromatic hydrocarbons (n-alkanes and PAHs) in remote areas, however, few studies have focused on those in the Tibetan Plateau. In this study, 18 pairs of atmospheric samples were obtained during the period from August 2006 to July 2007 in Lhasa, the capital city of Tibet. Both gas-phase and particulate-phase n-alkanes and PAHs were measured. Concentrations of n-alkanes (gas + particulate phase, 99.1–480.9 ng/m3) and PAHs (gas + particulate phase, 11.4–72.5 ng/m3) in Lhasa are lower than those in many cities. The sources of n-alkanes related to biological and petroleum sources were 67 and 33%, respectively. According to the results of diagnostic ratios and principal component analysis, emission of traffic vehicles was one of the important PAH sources, and sources of benzo(a)pyrene was likely attributed to incense burning. Good simulations were obtained by traffic soot-based model for fluoranthene, pyrene and benzo(a)anthracene, while, wood soot-based model fitted the experimental results of benzo(a)pyrene better. This meant atmospheric fate of PAHs was mainly influenced by the adsorptive partitioning that occurred during traffic and incense burning procedures. In addition, the benzo[a]pyrene-equivalent carcinogenic power (BaPE) in the present study (0.1–1.6 ng/m3) is lower than those in other cities and also the air quality standard of China, suggesting that atmospheric PAHs caused low health risks.  相似文献   

13.
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14.
Polycyclic aromatic hydrocarbons (PAHs) are a group of aromatic hydrocarbons with high toxicity to human health. PAH emissions from industrial activities have become the primary sources of PAH contamination in Chinese watersheds. Here, we analyzed 10 individual priority PAHs in 120 water samples taken from middle reach of Huaihe River, China. The results show that the PAH levels in studied watershed are significantly lower as compared to other Chinese watersheds, approaching or slightly exceeding the PAH levels in watersheds from selected European and North American countries. We observe rather large variation in spatial and vertical PAH distributions, pointing to PAH inputs from local industrial emissions, and PAH cycle among atmosphere, water and sediment. Individual PAH ratios (i.e., phenanthrene/anthracene and fluorene/pyrene) and principal components analysis suggest a primarily pyrolytic PAH sources (combustion of coal and coke) in water column. Other accompanying PAH sources include emissions from steel industry and gasoline. Total toxic benzo[a]pyrene equivalent of PAHs in studied water column indicates that PAHs in watershed of middle reach of Huaihe River pose limited toxicity to the environment.  相似文献   

15.
The concentration of selected contaminant trace metals and organic contaminants, namely polycyclic aromatic hydrocarbons (PAHs), normal-alkanes, total polychlorinated biphenyls (PCBs), and other organochlorines, was studied in cores from shallow-water fine-grain sediments from both sides of the maximum turbidity zone (MTZ) in the upper estuary of the St. Lawrence. Average trace metal concentrations in the cores were generally lower in downstream sediments, except for Hg and Pb. Hg levels in the cores were very high, exceeding 0.7 μg g?1 in core C168 (south shore) and 0.19 μg g?1 in core LE (north shore). Trace metal concentrations in all the cores were highly variable with depth, but after normalization with reference to iron, the trend was remarkably uniform, thus confirming an important inverse relationship with grain size. A similar lack of a well-defined trend was noted in the profiles of the organic components in the modern sediments. Average PAH values for modern sediments at core sites C168 and LO were 1.05 μg g?1 and 0.44 μg g?1, respectively (i.e., less than or equal to those in Lake Ontario and upstream in the river). PCB values far exceeded those in upstream sediments (average: 347 ng g?1 in core LE and 158 ng g?1 in C168), but were less than in Lake Ontario. Concentrations of chlordane, heachlorobenzene, and mirex were relatively low and uniform in the modern sections of the cores. The vertical uniformity of both the contaminant profiles and those for Cs-137 (C168) suggests that the sediments are relatively young (i.e., definitely less than 35 yr at C168, and probably even less at LE and LO). Therefore no long-term or historical trend is evident.  相似文献   

16.
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   

17.
A new and significant site of organic silty sand has been found beneath the Valders till at Valders Quarry in northeastern Wisconsin. This is now the earliest known late-glacial site associated with red till ice advances in the western Great Lakes area. Leaves of terrestrial plants washed into a small depression provide a date of 12,965 ± 200 yr B.P. (WIS-2293), which is significantly older than the Two Creeks Forest Bed (ca. 11,800 yr B.P.). Percentage and concentration pollen diagrams suggest that the site was open and distant from a closedPiceaforest. No wood orPiceaneedles have been found. This date is statistically indistinguishable from 12,550 ± 233 yr B.P., the mean of three dates for the end of inorganic varve sedimentation at Devils Lake, 160 km southwest at the terminus of the Green Bay Lobe. Assuming that the Green Bay lobe vacated its outermost moraine in the interval from 13,000 to 12,500 yr B.P., only a short time was available for retreat of the ice margin over 350 km, drainage of red sediment from Lake Superior into the Lake Michigan basin, readvance of over 250 km, retreat of at least 80 km, and advance to this site. The time for these events appears to have been too short to resolve by current radiocarbon technique. This extremely rapid collapse of the Green Bay lobe has a calibrated age of about 15,000 cal yr B.P., about that of the dramatic warming seen in the Greenland ice cores.  相似文献   

18.
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   

19.
Karst areas have much higher ecological vulnerability and are easy to be contaminated by polycyclic aromatic hydrocarbons (PAHs), which are introduced as health risk pollutants. PAHs ratios were used to understand the sources and transport behavior of PAHs conducted in the karst Nanshan Underground River, China. Water, sediments from the underground river and water, sediments, soil from the surface were collected monthly in 2011 and 2012. Abundant PAHs were found both in the underground river and in the surface system. The detected ΣPAHs concentrations varied from 353 to 13,203 ng L?1 in the groundwaters and content from 169 to 12,038 ng g?1 in the sediments of the underground river. The ratios of anthracene to anthracene, plus phenanthrene and fluoranthene to fluoranthene, plus pyrene indicated that PAHs were delivered in the groundwaters from combusted grass, wood, and coal, while in the sediments were a mixture of non-combusted petroleum, grass, wood, coal and combusted grass, wood, coal. The similarities in sources between an underground river and surface system indicated that farmlands play a major role for the transport of PAHs and contamination in the underground river. Karst features are liable for the transport behavior.  相似文献   

20.
Total organic carbon (TOC), Total nitrogen (TN) and the phosphorus species concentrations of sediment cores taken from Zhushan Bay, Meiliang Bay, and East Taihu Lake regions in Taihu Lake, a large shallow lake in China, were determined. Experimental results showed a conspicuous eutrophication trend in the northern area of Taihu Lake. Inorganic P was found to be the main phosphorus form. Fe-bound P accounted for the largest proportion of Inorganic P in Meiliang Bay, an alga-type lake region. In East Taihu Lake, a macrophytic lake region, Ca-bound P was found in higher proportions than in other lake regions, with Organic P present in similarly large proportions. With respect to Taihu Lake sediment cores, the date at approximately 20 cm layer depth was roughly identified as 1950s, while upper 5 cm layers corresponded to the turn of the century. The drastic increase in phosphorus species concentration except for Ca-bound P was indicative of the large quantities of effluent discharge into Zhushan Bay owing to the increased industrial and agricultural production from the 1950s onwards. TN, Inorganic P, Organic P, and total phosphorus (TP) concentrations increased by over 2, 2.5, 2 and 2.5-fold, respectively, over the past five decades. A large proportion of Organic P accounted for TP, and high C/N ratios indicated that East Taihu Lake can be properly classified as an oligotrophic lake.  相似文献   

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