首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 624 毫秒
1.
Ko FC  Baker J  Fang MD  Lee CL 《Chemosphere》2007,66(2):277-285
Polycyclic aromatic hydrocarbon (PAH) concentrations in 34 surface sediments along the Susquehanna River were investigated in 2000. The total concentrations of PAHs in the surface sediments of Lake Clarke, Lake Aldred, the upper Conowingo Reservoir, and the lower Conowingo Reservoir were 3.3+/-1.5 microg g-1 (n=9), 1.6+/-1.3 microg g-1 (n=4), 9.8+/-5.5 microg g-1 (n=7), and 4.0+/-1.2 microg g-1 (n=14), respectively. These represent the first comprehensive measurement of PAHs in Susquehanna River surface sediments. Overall, total PAH concentrations were relatively lower in Lake Aldred, which is more shallow and sloped, and significantly higher in the upper Conowingo Reservoir. The sediment PAH levels were related to river flow rates, which are indirectly correlated with the particle size of the surface sediments. Total PAH levels in all the studied sites were below the effects range median (ERM) of 44.8 microg g-1 with 38% (13 of the 34 sampling sites) exceeding the effects range low (ERL) of 4.02 microg g-1. Principal component analysis indicated that variations in the PAH compound patterns of each reservoir decreased from upstream to downstream, indicating that the surface sediments were mixed along the Susquehanna River. The PAH patterns in the lower Conowingo Reservoir sediments were a combination of those upstream sources. Source analysis using isomer ratios as indicators suggested that PAHs in the Susquehanna River surface sediment are derived from the combustion of fossil fuels such as coal and gasoline with coal as the major source of contaminants.  相似文献   

2.
Honda K  Mizukami M  Ueda Y  Hamada N  Seike N 《Chemosphere》2007,68(9):1763-1771
The residue level of 21 polycyclic aromatic hydrocarbons (PAHs) and the temporal changes in this level were investigated in paddy soils collected from particular experimental sites in Japan from 1959 to 2002. The average total PAH concentration in all the samples was 496 microg kg(-1), and it ranged from 52.9 to 2180 microg kg(-1). The residue level of the PAHs was the highest during the 1960s, rapidly decreased during the 1970s, and remained almost constant thereafter. Relatively high PAH concentrations were observed in soils from areas that experienced heavy snowfall and that had relatively low air temperature. The predominant PAHs were phenanthrene, fluoranthene, naphthalene, and pyrene, and their concentration overall and in relation to that of the total PAHs decreased each year since the 1960s. Similarities in the PAH profiles among the locations were determined using the concentration correlation matrix and cluster analysis, and ratios of the levels of specific PAH pairs were also calculated to determine their origin. The collected data suggested that the origins of soil PAHs changed chronologically from the burning of agricultural wastes such as stubble before the mid-1970s to the combustion of fossil fuel and its secondary products after the mid-1970s.  相似文献   

3.
Oren A  Chefetz B 《Chemosphere》2005,61(1):19-29
Sorption and desorption behaviors of phenanthrene and naphthalene were studied with the whole sediment, humic acid (HA) and humin samples from downstream and upstream sites along the Kishon River, Israel. The 13C nuclear magnetic resonance spectra and the sorption coefficients suggest that sorption occurs to both aromatic and aliphatic moieties of the sedimentary organic matter and that rigid paraffinic domains probably contribute to the sorption non-linearity. The carbon-normalized Freundlich affinity values for the two sorbates were significantly higher for the whole sediment and humin samples from the downstream region of the river than for the upstream sediment samples. On the basis of the measured affinity values, the sorbents can be arranged in the following order: humin>HA>whole sediment. Phenanthrene exhibited the lowest desorption from the whole sediment samples compared with the other sorbents. For naphthalene, the desorption hysteresis obtained with the whole sediment and humin samples were similar: both exhibited a decrease in desorption with decreasing solute concentration. The higher sorption affinities observed for all the organic fractions from the downstream sediment are suggested to be related to the low levels of polar domains and humin content. It is concluded that in bulk sediment samples, the overall contribution of the HA fraction to short-term sorption is of high importance, but the sorption non-linearity is controlled mainly by the humin complexes. The low desorption potential recorded for the whole sediment samples could affect the natural attenuation of the sorbed hydrophobic organic compounds.  相似文献   

4.
Xia XH  Yu H  Yang ZF  Huang GH 《Chemosphere》2006,65(3):457-466
The contamination of polycyclic aromatic hydrocarbons (PAHs) has become one of the major problems in the Yellow River of China. As the Yellow River is the most turbid large river in the world, it remains unknown to which extent the high suspended sediment content in the river may affect the fate and effect of PAHs. Here we report the effect of sediment on biodegradation of chrysene, benzo(a)pyrene and benzo(g,h,i)perylene with phenanthrene as a co-metabolism substrate in natural waters from the Yellow River. Biodegradation kinetics of the PAHs in the river water with various levels of sediment contents were studied in the laboratory by fitting with a biodegradation kinetics model for organic compounds not supporting growth. The results indicated that the biodegradation rates of PAHs increased with the sediment content in the water. When the sediment contents were 0, 4 and 10 g/l, the biodegradation rate constants of chrysene with the initial concentration of 3.80 microg/l were 0.053, 0.084 and 0.111 d(-1), respectively. Further studies suggested the enhanced biodegradation rate in the presence of sediment was caused by the following mechanisms: (1) the population of PAH-degrading bacteria in the water system was found to increase with the sediment content; the bacteria population on sediment phase was far greater than that on water phase during the cultivation process; (2) the sorption of PAHs on the sediment phase was well described by the dual adsorption-partition model. Although the sorption capacity of PAH per unit weight of sediment decreased with the increase of the sediment content, the amount of sorbed PAH increased with the sediment content; and, (3) the desorption of PAHs from the solid phase led to a higher concentration near the water-sediment interface. Since the bacteria were also attached to the interface, this resulted in an increased contact chance between the bacteria and PAHs.  相似文献   

5.
Polycyclic aromatic hydrocarbons (PAH) were analysed in 23 soil samples (0–10 cm layer) from the Swiss soil monitoring network (NABO) together with total organic carbon (TOC) and black carbon (BC) concentration, as well as some PAH source diagnostic ratios and molecular markers. The concentrations of the sum of 16 EPA priority PAHs ranged from 50 to 619 μg/kg dw. Concentrations increased from arable, permanent and pasture grassland, forest, to urban soils and were 21–89% lower than median numbers reported in the literature for similar Swiss and European soils. NABO soils contained BC in concentrations from 0.4 to 1.8 mg/g dw, except for two sites with markedly higher levels. These numbers corresponded to 1–6% of TOC and were comparable to the limited published BC data in soil and sediments obtained with comparable analytical methods. The various PAH ratios and molecular markers pointed to a domination of pyrogenically formed PAHs in Swiss soils. In concert, the gathered data suggest the following major findings: (1) gas phase PAHs (naphthalene to fluorene) were long-range transported, cold-condensated at higher altitudes, and approaching equilibrium with soil organic matter (OM); (2) (partially) particle-bound PAHs (phenanthrene to benzo[ghi]perylene) were mostly deposited regionally in urban areas, and not equilibrated with soil OM; (3) Diesel combustion appeared to be a major emission source of PAH and BC in urban areas; and (4) wood combustion might have contributed significantly to PAH burdens in some soils of remote/alpine (forest) sites.  相似文献   

6.
Tremblay L  Kohl SD  Rice JA  Gagné JP 《Chemosphere》2005,58(11):302-1620
The impact of the lipid fraction of natural geosorbents on the sorption of a polycyclic aromatic hydrocarbon was assessed using several experiments. In the first set of experiments phenanthrene was sorbed on a coastal sediment as well as on its humin and humic acid fractions before and after lipid extraction. Before lipid extraction, sorption shows dominantly partitioning characteristics. However, the extraction of lipids from sediment and humin drastically increases, by up to one order of magnitude, their sorption affinity for phenanthrene at low sorbate concentrations, resulting in increased isotherm nonlinearity. This effect is less pronounced for humic acids. One mechanism proposed for the increasing sorption is that lipids, despite their very low relative abundance in the sediments, can compete with phenanthrene for specific high affinity sorption sites (e.g., matrix pores and adsorption sites). This competition is not surprising considering the similar hydrophobic nature of lipids and phenanthrene. Lipids, or any non-polar molecules, could also act like plasticizers by swelling rigid domains and disrupting high affinity sites. In both cases, the removal of lipids (and extraction solvents) makes those sites available for phenanthrene. These provide alternative explanations to the previously proposed “solvent conditioning effect” believed to occur when geosorbents are treated with non-polar solvents modifying the matrix structure, an effect yet to be proven at molecular scale. To further investigate the impact of lipids on sorption, other independent experiments were performed. In a second experiment, re-addition of lipids to the extracted sediment restored the sorption isotherm linearity observed in the native material supporting the absence of irreversible extraction artifacts. However, high addition of lipids (i.e., after saturation of high affinity sites) seems to also enlarge the low affinity partitioning domain. These results are consistent with dual-mode, hole-filling, sorption models involving diffusion. In the final set of experiments, solid-state 19F-NMR using F-labeled lipids sorbed onto the sediments confirmed that lipids may be in different domains (mobile or rigid) that interact or not with phenanthrene. The possible effects of lipid removal on sorption have been overlooked and should be considered when geosorbents are pretreated.  相似文献   

7.
In order to contain the movement of organic contaminants in groundwater, a subsurface sorption barrier consisting of sand or clay minerals coated with a cationic surfactant has been proposed. The effectiveness of such a sorption barrier might be affected by the presence of dissolved organic matter (DOM) in the groundwater. To study the impact of DOM on barrier performance, a series of batch experiments were performed by measuring naphthalene and phenanthrene sorption onto sand coated with cetylpyridinium chloride (CPC) and bentonite coated with hexadecyltrimethylammonium bromide (HDTMA) in the presence of various concentrations of DOM. The overall soil-water distribution coefficient (K*) of naphthalene and phenanthrene onto CPC-coated sand decreased with increasing DOM concentration, whereas the K* of the compounds onto HDTMA-coated bentonite slightly increased with increasing DOM concentration. To describe the overall distribution of polycyclic aromatic hydrocarbons (PAHs) in the systems, a competitive multiphase sorption (CMS) model was developed and compared with an overall mechanistic sorption (OMS) model. The modeling studies showed that while the OMS model did not explain the CPC-coated sand experimental results, a model that included competitive sorption between DOM and PAH did. The experimental results and the modeling study indicated that there was no apparent competition between DOM and PAH in the HDTMA-coated bentonite system, and indicated that in groundwater systems with high DOM, a barrier using HDTMA-coated bentonite might be more effective.  相似文献   

8.
Along 10 campaigns, from June 2002 to September 2004, the concentrations of 16 polycyclic aromatic hydrocarbons (PAHs) were measured in sediments and oysters (Crassostrea sp.) taken from four sites in the Unesco protected natural reserve of Urdaibai (Basque Country, Bay of Biscay). Total PAH concentration ranged from 0.7 to 140 microg kg(-1) (dw) in the case of sediments, and from 300 to 1400 microg kg(-1) (dw) in the case of oysters. During this study, the coast of the Bay of Biscay was severely affected by the Prestige oil spill (November 2002). Presumably, as a consequence of this accident, both spatial and temporal variations of the PAHs, as well as the sources of the PAHs were affected by the oil spill, and this effect was observed in the total concentrations and, especially, in several diagnostic ratios and in multivariate data analysis. Finally, both BAF (bioaccumulation factor) and BSAF (biota-sediment accumulation factor) parameters were calculated to conclude that particulate matter seems to be the most favourable uptake pathway of PAHs in oysters from this estuary.  相似文献   

9.
The spatial distribution, composition, and sources of polycyclic aromatic hydrocarbons (PAHs) in sediments and suspended particulate matter (SPM) from the Pearl River Estuary and adjacent coastal areas were examined. Total PAH concentrations varied from 189 to 637 ng/g in sediments and 422 to 1,850 ng/g in SPM. PAHs were dominated by 5,6-ring compounds in sediments and by 2,3-ring compounds in SPM samples. Assessment of PAH sources suggested that biomass and coal combustion is the major PAH source to the outer part of the estuary sediments and that petroleum combustion is the major PAH source to the inner part of estuary sediments. As for SPM samples, PAH isomer pair ratios indicated multiple (petroleum, petroleum combustion, and biomass and coal combustion) PAH sources, and significant temporal variations could exist for the sources of water column PAHs in the study area. The distribution of perylene in SPM samples indicated that the river was the dominant source of perylene in SPM and that perylene could be taken as an index to assess the contribution of river inflow to the total PAHs in SPM samples. The high concentration of perylene in the sediment was indicative of an in situ biogenic origin.  相似文献   

10.
The concentrations of total polycyclic aromatic hydrocarbons (sigmaPAHs) and 15 individual PAH compounds in 20 surface sediments collected from four mangrove swamps in Hong Kong were analysed. sigmaPAH concentrations ranged from 356 to 11,098 ng g(-1) dry weight with mean and median values of 1992 and 1,142 ng g(-1), respectively. These values were significantly higher than those of marine bottom sediments of Hong Kong harbours, suggesting that more PAHs were accumulated in mangrove surface sediments. The concentrations of sigmaPAHs as well as individual PAH compound varied significantly among mangrove swamps. The swamps heavily polluted by livestock and industrial sewage, such as Ho Chung and Mai Po, had much higher concentrations of total PAHs and individual PAH than the other swamps. The PAH profiles were similar among four mangrove swamps, and were dominated by naphthalene (two-ring PAH), fluorene and phenanthrene (three-ring PAH). The mangrove sediments had higher percentages of low-molecular-weight PAHs. These indicated that PAHs in mangrove sediments might originate from oil or sewage contamination (petrogenic input). Ratio values of specific PAH compounds such as phenanthrene/anthracene and fluoranthene/ pyrene, were calculated to evaluate the possible source of PAH contamination in mangrove sediments. These ratios varied among samples, suggesting that mangrove sediments might have a mixed pattern of pyrolytic and petrogenic inputs of PAHs. Sediments collected from Ho Chung mangrove swamp appeared to be more dominated by pyrolytic input while those from Tolo showed strong petrogenic contamination.  相似文献   

11.
Distributions of total organic carbon (TOC), black carbon (BC), and polycyclic aromatic hydrocarbons (PAH) were investigated in different particle size fractions for four Norwegian harbor sediments. The total PAH (16-EPA) concentrations ranged from 2 to 113 mg/kg dry weight with the greatest fraction of PAH mass in the sand fraction for three of the four sediments. TOC contents ranged from 0.84% to 14.2% and BC contents from 0.085% to 1.7%. This corresponds to organic carbon (OC = TOC - BC) contents in the range of 0.81-14% and BC:TOC ratios of 1.3-18.1%. PAH isomer ratios suggested that the PAH in all four sediments were of pyrogenic origin. Furthermore, stronger correlations between PAH versus BC (r2 = 0.85) than versus OC (r2 = 0.15) were found. For all size fractions and bulk sediments, the PAH-to-BC ratios for the total PAHs were on average 6+/-3 mg PAH/g BC. These results suggest that PAH distributions were dominated by the presence of BC, rather than OC. As sorption to BC is much stronger than sorption to OC, this may result in significantly lower dissolved concentrations of PAH than expected on the basis of organic carbon partitioning alone.  相似文献   

12.
Polycyclic aromatic hydrocarbons (PAHs) in a sediment core taken from intertidal flat in the Yangtze Estuary were determined by gas chromatography-mass spectrometry. The results indicate that the total concentration of PAHs ranged from 0.08 to 11.74 microg/g. The concentration levels of total and individual PAHs changed dramatically with depth. The concentrations of PAHs were relatively high above 35 cm depth and remained constantly low below this depth. The historical record of PAHs in the core shows subsurface maximum (one or more peak values), followed by decreased levels to the surface and with depth. And, PAH sediment record in the core profile is in agreement with historically sewage discharge events during the 1980s to 1990s. The distribution of target molecule acenephthene, the fluoranthene/pyrene ratio, the proportion of 2-3-ring and 4-5-ring PAHs, and alkylated naphthalene to parent naphthalene in the core profile show that the sources in this area are characterized by petroleum-derived PAH contamination (mainly sewage discharge and the river runoff) and the incorporation of atmospheric inputs. Studies indicate the PAH profile pattern in this site in comparison with other regions appear to reflect its particular local position (near the sewage outlet). Moreover, physico-chemical conditions and sedimentation rate as well as biodegradation also affect the PAH concentration levels in the core sediments.  相似文献   

13.
Surface soil (0-20 cm) samples from nine representative vegetable fields located in Guangzhou, Shenzhen, Zengcheng and Huadu within the Pearl River Delta, South China were collected and analyzed for 16 USEPA priority polycyclic aromatic hydrocarbons (PAHs) using gas chromatography coupled to mass spectrometry (GC-MS). Total concentrations of 16 PAHs (Sigma(PAHs)) ranged from 160 to 3700 microg kg(-1). Large variations were observed also between concentrations of individual PAHs from different vegetable fields and within the site as well. Acenapthylene, benzo[b]fluoranthene, fluoranthene, benzo[a]pyrene and benzo[k]fluoranthene were consistently the most prevalent individual PAHs. The values of PAH isomer ratios [anthracene/(anthracene+phenanthrene) and fluoranthene/(fluoranthene+pyrene)] indicate that combustion processes are the major sources of PAHs. Concentrations of PAHs were poorly correlated with organic carbon concentrations of soils, suggesting different sources and also indicating that the PAH pollution of this area is recent. The same outcome is confirmed by the predominance of PAHs with fewer rings (相似文献   

14.
The levels and distribution of polynuclear aromatic hydrocarbons (PAHs) were determined in soil samples from background locations in the UK and Norway, to investigate their spatial distribution and the controlling environmental factors. Concentrations ranged between 42 and 11200 microg kg(-1) (geometric mean 640 microg kg(-1)) and 8.6 and 1050 microg kg(-1) (150 microg kg(-1)) dry weight in the UK and Norwegian soil, respectively. Proximity to sources and locations susceptible to high atmospheric depositional inputs resulted in higher concentrations. Statistically significant relationships were observed between PAH and total organic carbon (TOC) in the Norwegian samples. High molecular weight PAHs correlated with black carbon (BC) in UK-woodland soil. These observations support the hypothesis that TOC plays an important role in the retention of PAHs in soil and that PAHs are often combined with BC during combustion emissions. PAHs with 4 and more rings comprised approximately 90% of total PAHs in the UK soil, but only 50% in the Norwegian soil. The mixture of PAHs implied that fractionation occurred during long-range atmospheric transport and deposition. The lighter PAHs with lower K(ow) values more readily reached the most remote sites. The heavier PAHs with higher K(ow) values remained in closer proximity to sources.  相似文献   

15.
Analytical techniques used to assess the environmental risk of contamination from polycyclic aromatic hydrocarbons (PAHs) typically consider only abiotic sample parameters. Supercritical fluid extraction and sorption enthalpy experiments previously suggested slow desorption rates for PAH compounds in two coal-contaminated floodplain soils. In this study, the actual PAH availability for aerobic soil microorganisms was tested in two series of soil-slurry experiments. The experimental conditions supported microbial degradation of phenanthrene if it was weakly sorbed onto silica gel. Native coals and coal-derived particles in two soils effectively acted as very strong sorbents and prevented microbial PAH degradation. The long history of PAH exposure and degree of coal contamination apparently had no influence on the capability of the microbial soil community to overcome constraints of PAH availability. Within the context of the experimental conditions and the compounds chosen, our results confirm that coal-bound PAHs are not bioavailable and hence of low environmental concern.  相似文献   

16.
Polycyclic aromatic hydrocarbons (PAHs) were quantified in 30 soil profiles from the Yangtze River Delta Region, in east China. Relative concentrations of PAH compounds with different benzene rings and ratios of fluoranthene to fluoranthene plus pyrene and benz(a)anthracene to benz(a)anthracene plus chrysene were used to identify the possible sources of soil PAHs. Total concentrations of 15 PAHs in topsoils ranged from 8.6 to 3881 microg kg(-1) with an average of 397 microg kg(-1). Half of the soil samples were considered to be contaminated with PAHs (>200 microg kg(-1)) and two sampling sites were heavily polluted by PAHs with concentrations >1000 microg kg(-1). Phenanthrene was found in soils below a depth of 100 cm in half of the sampling sites, but the detectable ratio of benzo(a)pyrene decreased sharply from 100% in topsoil to 0 in the 4th horizon.  相似文献   

17.
Effect of rhamnolipids on the uptake of PAHs by ryegrass   总被引:7,自引:0,他引:7  
A hydroponic experiment was conducted to investigate the effect of rhamnolipids, a biosurfactant, on the uptake of polycyclic aromatic hydrocarbons (PAHs) by ryegrass. Results showed that rhamnolipids could enhance the uptake of PAHs by ryegrass roots. With increasing concentration of rhamnolipids, the PAH content in ryegrass roots initially increased and then decreased, while the PAH content in ryegrass shoots did not change. Batch studies also showed that the sorption of phenanthrene by fresh ryegrass roots was dependent on rhamnolipid concentration and showed the same trends as the uptake experiment. The increase of permeability of ryegrass root cells with the increase of rhamnolipid concentration may lead to the initial enhancement of PAH content in ryegrass roots, and the decrease of PAH adsorption onto the root surface with further increase of rhamnolipids led to the decrease of PAH content in ryegrass roots.  相似文献   

18.
A batch experiment was conducted to compare PAH degradation in a polluted river sediment under aerobic and anaerobic conditions, and to investigate whether input of fresh organic material (cellulose) could enhance such degradation. All measurements were checked against abiotic control treatments to exclude artifacts of sample preparation and non-biological processes like aging. Three- and four-ring PAHs could be degraded by the indigenous microbial community under aerobic conditions, but anaerobic metabolism based on iron and sulphate reduction was not coupled with PAH degradation of even the simplest 3-ring compounds like phenanthrene. Cellulose addition stimulated both aerobic and anaerobic respiration, but had no effect on PAH dissipation. We conclude that natural attenuation of PAHs in polluted river sediments under anaerobic conditions is exceedingly slow. Dredging and biodegradation on land under aerobic conditions would be required to safely remediate and restore polluted sites.  相似文献   

19.
Krauss M  Wilcke W 《Chemosphere》2005,59(10):1507-1515
The sorption strength of persistent organic pollutants in soils may vary among different soil organic matter (SOM) pools. We hypothesized that polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) were unevenly distributed and had different soil organic carbon (SOC)-water partition coefficients (K(OC)) among soil density fractions. We determined the concentrations and K(OC) values of 20 PAHs and 12 PCBs in bulk samples and three density fractions (light, <2.0, medium, 2.0-2.4, and heavy, >2.4 g cm(-3)) of 11 urban topsoils (0-5 cm) from Bayreuth, Germany. The K(OC) values were determined using sequential extraction with methanol-water mixtures (35% and 65% methanol) at 60 degrees C. The sum of 20 PAH concentrations in bulk soil ranged 0.4-186 mg kg(-1), and that of 12 PCB concentrations 1.2-158 microg kg(-1). The concentrations of all PAHs and PCBs decreased in the order light>medium>heavy fraction. When normalized to the SOC concentrations, PAH concentrations were significantly higher in the heavy than in the other density fractions. The K(OC) values of the PAHs in density fractions were 3-20 times higher than those of the PCBs with similar octanol-water partition coefficients (K(OW)). The K(OC) values of individual PAHs and PCBs varied up to a factor of 1000 among the studied soils and density fractions. The K(OC) values of 5- and 6-ring PAHs tended to be highest in the heavy fraction, coinciding with their enrichment in this fraction. For the other PAHs and all PCBs, the K(OC) values did not differ among the density fractions. Thus, there is no relationship between sorption strength and distribution among density fractions, indicating that density fractionation is not a suitable tool to distinguish among differently reactive PAH and PCB pools in soils.  相似文献   

20.
Polycyclic aromatic hydrocarbon (PAH) concentrations were measured in Pontoporeia hoyi, the most abundant benthic organism in Lake Michigan, and in its associated sediment/pore water matrix. Individual PAH concentrations ranged from 10 ppb to 1 ppm in three sedimentary environments having different levels of organic carbon. Pore water concentrations appeared to be independent of sediment concentrations. P. hoyi bioconcentration factors ranged from approximately 104 to 105 for seven analyzed PAHs. A major fraction of the phenanthrene, fluoranthene and pyrene in P. hoyi appears to come from sediments and pore water, while chrysene and BaP are primarily obtained from water.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号