Distribution and sources of polycyclic aromatic hydrocarbons (PAHs) in sediment from the upper reach of Huaihe River,East China

Introduction  

To assess the status of polycyclic aromatic hydrocarbons (PAHs) contamination in sediments from the upper reach of Huaihe River, East China, 16 surface sediment samples were collected in March 2007 and analyzed for 16 USEPA priority PAHs.     

Source apportionment of polycyclic aromatic hydrocarbons in surface sediments of the Bohai Sea, China

A total of 112 surface sediment samples covering virtually the entire Bohai Sea were analyzed for polycyclic aromatic hydrocarbons (PAHs), in order to provide the extensive information of recent occurrence levels, distribution, possible sources, and potential biological risk of these compounds in this area. Surface sediment samples were collected from the Bohai Sea using a stainless steel grab sampler. Sixteen PAHs were determined by a Finnigan TRACE DSQ gas chromatography/mass spectrometry. Diagnostic ratios, cluster analysis, and principal component analysis (PCA) with multivariate linear regression (MLR) were performed to identify and quantitatively apportion the major sources of sedimentary PAHs in the Bohai Sea. Concentrations of total PAHs in the Bohai Sea ranged widely from 97.2 to 300.7 ng/g (mean, 175.7?±?37.3 ng/g). High concentrations of PAHs were found in the vicinity of Luan River Estuary-Qinhuangdao Harbor, Cao River Estuary-Bohai Sea Center, and north of the Yellow River Estuary. The three-ring PAHs were most abundant, accounting for about 37?±?5 % of total PAHs. The four-ring and five-ring PAHs were the next dominant ones comprising approximately 29?±?7and 23?±?3 % of total PAHs, respectively. Concentrations of acenaphthylene, acenaphthene, and dibenz[a,h]anthracene are higher than Canadian interim marine sediment quality guideline values at most of the sites in the study area. Contamination levels of PAHs in the Bohai Sea were low in comparison with other coastal sediments in China and developed countries. The distribution pattern of PAHs and source identification implied that PAH contamination in the Bohai Sea mainly originates from petrogenic and pyrogenic sources. Further PCA/MLR analysis suggested that the contributions of spilled oil products (petrogenic), coal combustion, and traffic-related pollution were 39, 38, and 23 %, respectively. Pyrogenic sources (coal combustion and traffic-related pollution) contributed 61 % of anthropogenic PAHs to sediments, which indicates that energy consumption could be a dominant factor in PAH pollution in this area. Acenaphthylene, acenaphthene, and dibenz[a,h]anthracene are the three main species of PAHs with more ecotoxicological concern in the Bohai Sea.     

Source apportionment and source/sink relationships of PAHs in the coastal atmosphere of Chicago and Lake Michigan

Multivariate statistical techniques were used to investigate source apportionment and source/sink relationships for polycyclic aromatic hydrocarbons (PAHs) in the urban and adjacent coastal atmosphere of Chicago/Lake Michigan in 1994–1995. The PAH signatures for the atmospheric particle phase, surface water particle phase and sediments indicate that atmospheric deposition is the major source of PAHs to the sediments and water column particulate phase of Lake Michigan. The PAH signature for the atmospheric gas phase and water dissolved phase indicate an intimate linkage between the lake and its overlying atmosphere. A modified factor analysis-multiple regression model was successfully applied to the source apportionment of atmospheric PAHs (gas+particle). Coal combustion accounted for 48±5% of the ΣPAH concentration in both the urban and adjacent coastal atmosphere, natural gas combustion accounted for 26±2%, coke ovens accounted for 14±3%, and vehicle emissions (gas+diesel) accounted for 9±4%. Each is an identified source category for the region. These results are consistent with the mix of fossil fuel combustion sources and ratios of indicator PAHs.     

Seasonal variation and source estimation of organic compounds in urban aerosol of Augsburg, Germany

This study reports a general assessment of the organic composition of the PM_2.5 samples collected in the city of Augsburg, Germany in a summer (August-September 2007) and a winter (February-March 2008) campaign of 36 and 30 days, respectively. The samples were directly submitted to in-situ derivatisation thermal desorption gas chromatography coupled with time of flight mass spectrometry (IDTD-GC-TOFMS) to simultaneously determine the concentrations of many classes of molecular markers, such as n-alkanes, iso- and anteiso-alkanes, polycyclic aromatic hydrocarbons (PAHs), oxidized PAHs, n-alkanoic acids, alcohols, saccharides and others.The PCA analysis of the data identified the contributions of three emission sources, i.e., combustion sources, including fossil fuel emissions and biomass burning, vegetative detritus, and oxidized PAHs. The PM chemical composition shows seasonal trend: winter is characterized by high contribution of petroleum/wood combustion while the vegetative component and atmospheric photochemical reactions are predominant in the hot season.     

Occurrence and assessment of polycyclic aromatic hydrocarbons in soils from vegetable fields of the Pearl River Delta, South China

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   

Composition and distribution of polycyclic aromatic hydrocarbons in the surface sediments from the Susquehanna River

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.     

One century sedimentary records of polycyclic aromatic hydrocarbons, mercury and trace elements in the Qinghai Lake, Tibetan Plateau

Sediments from a remote lake of northeastern Tibetan Plateau were analyzed for polycyclic aromatic hydrocarbons (PAHs) and trace metals. USEPA priority PAHs, ranged from 11 in 1860 to 279 ng g⁻¹ in 2002, while, the deposition fluxes were in the range of 0.2-11.4 ng cm⁻² yr⁻¹. Similarly, from 1860 to 2002, an increased trend of Hg flux was observed (0.5-3.2 ng cm⁻² yr⁻¹). Remarkable increase of PAHs and Hg concentration began from 1970, nearly the same period of the “Reform and Open” Policy had been embarked (1978) in China. Good correlations were found between concentrations of Pb, Zn, Cd, As, Hg, and PAHs, which suggested the sources of these chemicals in the sediment is analogous, likely from anthroprogenic sources. Based on isomer ratios, PAHs in core were dominantly from the incomplete combustion of coal. Owing to the proximity to dust source area (Qaidam Basin) and the close association between PAHs, Hg, Pb, and particle matters, atmospheric dust-transport and deposition might be the main pathways that pollutants enter into Qinghai Lake.     

Emission factors and particulate matter size distribution of polycyclic aromatic hydrocarbons from residential coal combustions in rural Northern China

Coal consumption is one important contributor to energy production, and is regarded as one of the most important sources of air pollutants that have considerable impacts on human health and climate change. Emissions of polycyclic aromatic hydrocarbons (PAHs) from coal combustion were studied in a typical stove. Emission factors (EFs) of 16 EPA priority PAHs from tested coals ranged from 6.25 ± 1.16 mg kg^?1 (anthracite) to 253 ± 170 mg kg^?1 (bituminous), with NAP and PHE dominated in gaseous and particulate phases, respectively. Size distributions of particulate phase PAHs from tested coals showed that they were mostly associated with particulate matter (PM) with size either between 0.7 and 2.1 μm or less than 0.4 μm (PM_0.4). In the latter category, not only were more PAHs present in PM_0.4, but also contained higher fractions of high molecular weight PAHs. Generally, there were more than 89% of total particulate phase PAHs associated with PM_2.5. Gas-particle partitioning of freshly emitted PAHs from residential coal combustions were thought to be mainly controlled by absorption rather than adsorption, which is similar to those from other sources. Besides, the influence of fuel properties and combustion conditions was further investigated by using stepwise regression analysis, which indicated that almost 57 ± 10% of total variations in PAH EFs can be accounted for by moisture and volatile matter content of coal in residential combustion.     

Sediment-associated aliphatic and aromatic hydrocarbons in coastal British Columbia, Canada: concentrations, composition, and associated risks to protected sea otters

Sediment-associated hydrocarbons can pose a risk to wildlife that rely on benthic marine food webs. We measured hydrocarbons in sediments from the habitat of protected sea otters in coastal British Columbia, Canada. Alkane concentrations were dominated by higher odd-chain n-alkanes at all sites, indicating terrestrial plant inputs. While remote sites were dominated by petrogenic polycyclic aromatic hydrocarbons (PAHs), small harbour sites within sea otter habitat and sites from an urban reference area reflected weathered petroleum and biomass and fossil fuel combustion. The partitioning of hydrocarbons between sediments and adjacent food webs provides an important exposure route for sea otters, as they consume ∼25% of their body weight per day in benthic invertebrates. Thus, exceedences of PAH sediment quality guidelines designed to protect aquatic biota at 20% of the sites in sea otter habitat suggest that sea otters are vulnerable to hydrocarbon contamination even in the absence of catastrophic oil spills.     

Source Apportionment and Identification of Polycyclic Aromatic Hydrocarbons (PAHs) in Sediment Cores of Selected Creeks in Delta State,Nigeria

Polycyclic aromatic hydrocarbons (PAHs) seasonal variation and sources in Ubeji, Ifie, and Egbokodo Creeks of the Niger Delta, Nigeria, were predicted using diagnostic ratios (DRs) of parent PAHs (Phe/Phe + Ant; Flu/Flu + Pyr; BaA/BaA + Chry, and Ind/Ind + BghiP) and principal component analysis (PCA). A total of 222 sediment core samples were collected during the wet (August 2010) and the dry seasons (January 2011). The samples were dried and Soxhlet extracted; sample extracts were fractionated and analyzed by gas chromatography/flame ionization detection (GC/FID) to identify individual PAHs. The diagnostic PAH ratios revealed that PAHs in the sediment cores at the three creeks, in both seasons, mainly stemmed from the combustion process (pyrogenic sources). Principal component analysis further confirmed that wood-burning, coal combustion, diesel, gasoline-powered vehicular emissions, and petroleum combustion were the dominant contributors of PAHs sources at the sampling location. This study provided information on the origin and sources of PAHs in sediment cores, which may be useful for regulatory actions, environmental quality management, contamination history, and environmental forensic studies.     

Distribution of polycyclic aromatic hydrocarbons in surface water and sediment near a drinking water reservoir in Northeastern China

The levels of polycyclic aromatic hydrocarbons (PAHs) in the water and the sediment samples collected near the Mopanshan Reservoir—the most important drinking water resource of Harbin City in Northeast China—were examined. A total of 16 PAHs were concurrently identified and quantified in the three water bodies tested (Lalin River, Mangniu River, and Mopanshan Reservoir) and in the Mopanshan drinking water treatment plant during the high- and low water periods. The total PAH concentrations in the water and sediment samples ranged from 122.7 to 639.8 ng/L and from 89.1 to 749.0 ng/g dry weight, respectively. Similar spatial and temporal trends were also found for both samples. The lowest Σ₁₆PAH concentration of the Mopanshan Reservoir was obtained during the high water period; by contrast, the Lalin River had the highest concentration during the low water period. The PAH profiles resembling the three water bodies, with high percentages of low-molecular weight PAHs and dominated by two- to three-ring PAHs (78.4 to 89.0 %). Two of the molecular indices used reflected the possible PAH sources, indicating the main input from coal combustion, especially during the low water period. The conventional drinking water treatment operations resulted in a 20.7 to 67.0 % decrease in the different-ringed PAHs in the Mopanshan-treated drinking water. These findings indicate that human activities negatively affect the drinking water resource. Without the obvious removal of the PAHs in the waterworks, drinking water poses certain potential health risks to people.     

Spatial and temporal distribution of polycyclic aromatic hydrocarbons (PAHs) in surface water from Liaohe River Basin,northeast China

Liaohe River Basin is an important region in northeast China, which consists of several main rivers including Liao River, Taizi river, Daliao River, and Hun River. As a highly industrialized region, the basin receives dense waste discharges, causing severe environmental problems. In this study, the spatial and temporal distribution of aqueous polycyclic aromatic hydrocarbons (PAHs) in Liaohe River Basin from 50 sampling sites in both dry (May) and level (October) periods in 2012 was investigated. Sixteen USEPA priority PAHs were quantified by gas chromatography/mass selective detector. The total PAH concentration ranged from 111.8 to 2,931.6 ng/L in the dry period and from 94.8 to 2766.0 ng/L in the level period, respectively. As for the spatial distribution, the mean concentration of PAHs followed the order of Taizi River > Daliao River > Hun River > Liao River, showing higher concentrations close to large cities with dense industries. The composition and possible sources of PAHs in the water samples were also determined. The fractions of low molecular weight PAHs ranged from 58.2 to 93.3 %, indicating the influence of low or moderate temperature combustion process. Diagnostic ratios, principal component analysis, and hierarchical cluster analysis were used to study the possible source categories in the study area, and consistent results were obtained from different techniques, that PAHs in water samples mainly originated from complex sources, i.e., both pyrogenic and petrogenic sources. The benzo[a]pyrene equivalents (EBaP) characterizing the ecological risk of PAHs to the aquatic environment suggested that PAHs in Liaohe River Basin had already caused environmental health risks.     

Characterization of TSP-bound n-alkanes and polycyclic aromatic hydrocarbons at rural and urban sites of Tianjin, China

Total suspended particle (TSP) was collected and analyzed at rural and urban sites in Tianjin, China during the domestic heating season (from 15 November to 15 March) of 2003/4 for n-alkanes and 16 polycyclic aromatic hydrocarbons (PAHs). The normalized distribution of n-alkanes with the peak at C22, C23, C24 or C25 suggested that fossil fuel utilization was the major source of particulate n-alkanes at both sites. PAHs normalized distribution for each sample was similar and the higher molecular weight PAH dominated the profile (around 90%) indicating a stronger combustion source at both sites. Precipitation and wind were the most important meteorological factors influencing TSP and PAHs atmospheric concentrations. In the urban area the emission height had significant influence on PAHs levels at different heights under the relative stable atmospheric conditions. Coal combustion was the major source for TSP-bound PAHs at both sites based on some diagnostic ratios.     

Distribution of polycyclic aromatic hydrocarbons in the sediments of the Adriatic Sea

Distribution of the sixteen polycyclic aromatic hydrocarbons (PAHs) indicated from USEPA as priority pollutants was studied in surface sediments of two coastal areas of the Adriatic Sea. PAHs were recovered from the sediments by solvent extraction and then analyzed by means of gas chromatography-mass spectrometry. Total concentrations of the analytes in the range 24.1-501.1 ng/g were detected. The observed distribution has been discussed taking into account different aspects, such as the fluvial inputs and the grain size of the sediments. By using a molecular marker approach and characteristic compositional patterns it was possible to ascribe to combustion processes the main source of PAHs. Furthermore a good correlation between benzo[a]pyrene and the total concentration of PAHs (r=0.953) has been pointed out.     

Characterization and sources assignation of PM2.5 organic aerosol in a rural area of Spain

The results from a year-long study of the organic composition of PM2.5 aerosol collected in a rural area influenced by a highway of Spain are reported. The lack of prior information related to the organic composition of PM2.5 aerosol in Spain, concretely in rural areas, led definition of the goals of this study. As a result, this work has been able to characterize the main organic components of atmospheric aerosols, including several compounds of SOA, and has conducted a multivariate analysis in order to assign sources of particulate matter. A total of 89 samples were taken between April 2004 and April 2005 using a high-volume sampler. Features and abundance of n-alkanes, polycyclic aromatic hydrocarbons (PAHs), alcohols and acids were separately determined using gas chromatography/mass spectrometry and high performance liquid chromatography analysis. The Σn-alkane and ΣPAHs ranged from 3 to 81 ng m^?3 and 0.1 to 6 ng m^?3 respectively, with higher concentrations during colder months. Ambient concentrations of Σalcohols and Σacids ranged from 21 to 184 ng m^?3 and 39 to 733 ng m^?3, respectively. Also, several components of secondary organic aerosol have been quantified, confirming the biogenic contribution to ambient aerosol. In addition, factor analysis was used to reveal origin of organic compounds associated to particulate matter. Eight factors were extracted accounting more than 83% of the variability in the original data. These factors were assigned to a typical high pollution episode by anthropogenic particles, crustal material, plant waxes, fossil fuel combustion, temperature, microbiological emissions, SOA and dispersion of pollutants by wind action. Finally, a cluster analysis was used to compare the organic composition between the four seasons.     

Spatial and temporal distribution of polycyclic aromatic hydrocarbons (PAHs) in sediments from Daya Bay, South China

The spatial and temporal distribution of polycyclic aromatic hydrocarbons (PAHs) has been investigated in Daya Bay, China. The total concentration of the 16 USEPA priority PAHs in surface sediments ranged from 42.5 to 158.2 ng/g dry weight with a mean concentration of 126.2 ng/g. The spatial distribution of PAHs was site-specific and combustion processes were the main source of PAHs in the surface sediments. Total 16 priority PAH concentration in the cores 8 and 10 ranged from 77.4 to 305.7 ng/g and from 118.1 to 319.9 ng/g respectively. The variation of the 16 PAH concentrations in both cores followed the economic development in China very well and was also influenced by input pathways. Some of the PAHs were petrogenic in core 8 while pyrolytic source was dominant in core 10. In addition, pyrolytic PAHs in both cores were mainly from the coal and/or grass and wood combustion.     

Characterization,identification of road dust PAHs in central Shanghai areas,China

Road dust samples were collected from central Shanghai in winter (January) and summer (August), respectively. Sixteen polycyclic aromatic hydrocarbons (PAHs) in the United States Environmental Protection Agency (USEPA) priority-controlled list were determined by GC/MS. Total PAH (t-PAH) concentrations in winter samples ranged from 9176 to 32,573 ng g⁻¹ with a mean value of 20,648 ng g⁻¹, while they varied from 6875 to 27,766 ng g⁻¹ in summer with an average of 14,098 ng g⁻¹. Spatial variation showed that city park (CP) samples had the lowest t-PAH concentration, while industrial area (ID) and traffic area (TR) and commercial area (CO) were the most polluted, in both seasons. PAH homologues concentrations were getting higher with the more rings and higher molecular weight (HMW) in all areas. The study of effective factors showed that grain size was only a minor factor influencing the accumulation of PAHs, whereas total organic carbon (TOC) was found to be closely correlated with t-PAH concentration. Prevailing winds could directly affect on the spatial distribution of PAHs. Chemical source apportionment studies took the form of principal component analysis (PCA), followed by compositional analysis. It was demonstrated that road dust PAHs in central Shanghai mainly came from the mixing of traffic and coal combustion. The contribution percentages of pyrogenic and petrogenic sources were respectively 71.0% and 11.4% in winter, while they were, 64.9% and 14.1% in summer, respectively. Road dust PAHs in Shanghai city mostly came from local sources.     

Chemical characterization and source identification of polycyclic aromatic hydrocarbons in aerosols originating from different sources

To obtain the characteristic factors or signatures of particulate polycyclic aromatic hydrocarbons (PAHs) to help identify the sources of particulate PAHs in the atmosphere, different carbonaceous aerosols were generated by burning different fossil fuels and biomass under different conditions in the laboratory, and the chemical characteristics of 14 PAHs were studied in detail. The results showed that (1) carbonaceous aerosols derived from domestic burning of coal, diesel fuel, and gasoline have much higher concentrations of PAHs than those derived from domestic burning of biomass; (2) carbonaceous aerosols derived from domestic burning of diesel fuel/gasoline have similar PAH components as those derived from high-temperature combustion of diesel fuel/gasoline, although the former have much higher concentrations of PAHs than the latter, suggesting that the burning temperature obviously affects the emitting amount of particulate PAHs, but only slightly influences the PAHs components; and (3) the ratios of benzo[b]fluoranthene/acenaphthylene, benzo[b]fluoranthene/fluorene, dibenzo[a,h]anthracene/acenaphthylene, dibenzo[a,h]anthracene/fluorine, and benzo[b]fluoranthene/benzo[k]fluoranthene in carbonaceous aerosols are sensitively dependent on their sources, indicating that these ratios are suitable for use as characteristic factors or signatures of particulate PAHs in the atmosphere.     

Pressure-assisted ozonation of PCB and PAH contaminated sediments

Sediment contamination by recalcitrant organics such as polychlorinated biphenyls (PCBs) and polycyclic aromatic hydrocarbons (PAHs) is prevalent and of a great concern. Remediation efforts are hampered by the hydrophobic nature of the contaminants that limits their availability as well as by the sediment matrix that limits their exposure to treatment agents. Using contaminated sediment samples from the Passaic River, St. Louis River, Waukegan Harbor, and Wells National Estuarine Research Reserve, this research demonstrated a new ozonation technique that incorporates rapid, successive cycles of pressurization (690 kPa) and depressurization, enabling more effective treatment than conventional ozonation would. Conventional ozonation reached maximum 60% and 40% removal of PAHs from the Passaic River (40 mg kg(-1) initially) and St. Louis River sediment (520 mg kg(-1) initially), respectively, in 1h; however, removals ceased despite prolonged treatment for 2h. The pressure-assisted technique removed 96% of PAHs from both river sediments within 1h; it completely removed both PAHs (16 mg kg(-1) initially) and PCBs (5.1 mg kg(-1) initially) from the Waukegan Harbor sediment in 0.5 h. The heightened treatment is explained by soil aggregate fracturing upon pressure cycles that exposes the contaminants as well as by the confluence of hydrophobic contaminants and O(3) at the gas-liquid interface in the presence of microbubbles. The technique is expected to accelerate O(3) treatment of a wide range of organic contaminants, and it may provide treatment to dredged and stored contaminated sediment.     

Historical record of polycyclic aromatic hydrocarbons (PAHs) and spheroidal carbonaceous particles (SCPs) in marine sediment cores from Admiralty Bay, King George Island, Antarctica

This paper describes the first results of polycyclic aromatic hydrocarbons (PAHs) and spheroidal carbonaceous particles (SCPs) in sediment cores of Admiralty Bay, Antarctica. These markers were used to assess the local input of anthropogenic materials (particulate and organic compounds) as a result of the influence of human occupation in a sub-Antarctic region and a possible long-range atmospheric transport of combustion products from sources in South America. The highest SCPs and PAHs concentrations were observed during the last 30 years, when three research stations were built in the area and industrial activities in South America increased. The concentrations of SCPs and PAHs were much lower than those of other regions in the northern hemisphere and other reported data for the southern hemisphere. The PAH isomer ratios showed that the major sources of PAHs are fossil fuels/petroleum, biomass combustion and sewage contribution generally close to the Brazilian scientific station.