Concentrations, sources and temporal trends in atmospheric polycyclic aromatic hydrocarbons in a major conurbation

Concentrations of atmospheric PAH were separately determined in total suspended particulate matter and associated vapour phase in ambient air in Birmingham, UK. Samples of 24 h duration were taken simultaneously at two locations (the Bristol Road Observatory Site, BROS, and the Elms Road Observatory Site, EROS) on 44 separate occasions every one to two weeks between October 1999 and January 2001. BROS was 10 m from the busy Bristol Road, 800 m from EROS that was located within the "green space" of the University of Birmingham campus. With the exception of acenaphthene, average concentrations of all measured PAH at BROS exceed those at EROS, with a paired t-test revealing these roadside increments to be significant (p < 0.05) for 9 out of the 16 target PAH, demonstrating the importance of traffic emissions of PAH. Although the declines were not statistically significant (p > 0.05) except for phenanthrene and fluoranthene, concentrations of individual PAH at EROS between July and December inclusive in 1999 and 2000 fell by between 16 and 54% compared with those during the same months in 1997. Multiple linear regression of PAH concentrations against meteorological variables confirmed the influence of the Bristol Road on BROS but not EROS. Cluster analysis of PAH contamination in individual samples showed there to be two statistically distinct groups of samples. One group contained 15 samples, all of which displayed elevated concentrations. Examination of air mass back trajectory data, revealed that these PAH pollution episodes originate due to the combined effects of meteorology and local traffic emissions, rather than as a result of long-range transport. Eighteen 12 h samples were also taken at EROS over the period of the November Bonfire Night festivals of 1999 and 2000. These revealed significantly elevated PAH concentrations on the nights when ignition of bonfires and fireworks would be anticipated to peak. These results are relevant to assessments of the impact of similar "festivals of fire" elsewhere. In particular, retene (7-isopropyl-1-methylphenanthrene) concentrations were especially elevated, indicating it has possible utility as an indicator of wood combustion emissions.     

Spatial distribution and temporal trends of polycyclic aromatic hydrocarbons in Mytilus galloprovincialis from the Iberian Mediterranean coast

Polycyclic aromatic hydrocarbons (PAHs) have been determined in blue mussels (Mytilus galloprovincialis) from several Iberian Mediterranean coastal areas through the implementation of a monitoring programme from Spain in the framework of the Mediterranean Pollution Programme (MED POL). The selected areas correspond to sites with differing degrees of exposure to the main pollution sources (hot spots, coastal and reference areas). The sampling campaigns were performed from 2004 to 2009, with samples being taken from May to June, the non-spawning period for mussels in this area. Thirteen PAHs were determined by high-performance liquid chromatography with specific fluorescence detection. In general, total PAHs concentration was lower than 50 μg kg^?1 d.w., except in areas close to the principal ports and cities (Barcelona, Tarragona, Valencia and Algeciras) where it varies from 75 to 390 μg kg^?1 d.w. Background concentrations have been proposed for PAHs in mussels (23.8 μg kg^?1 d.w.) from Western Mediterranean area. Temporal trends were not statistically significant for PAHs concentrations from 2004 to 2009. Longer monitoring periods would be required to detect a continuous tendency, especially for PAHs because although the efficiency of combustion engines has reduced PAHs emissions, their increasing use could alter this potential reduction. The predominant PAHs were three and four ring congeners in all cases, with the predominance of phenanthrene in mussels sited far from the main PAHs sources. The phenanthrene/anthracene (lower than 10) and fluoranthene/pyrene (higher than 1) ratios indicate that PAHs detected in Spanish Mediterranean coastal mussels are mainly of pyrolytic origin.     

Particle-bound polycyclic aromatic hydrocarbons in an urban, industrial and rural area in the western Mediterranean

Particle-bound PAHs were measured at three sites in southeastern Spain (an urban background location, a suburban-industrial site in the vicinity of two cement plants and a rural area) in order to investigate the influence of the type of location on PAH concentrations. A clear influence of cement production on particulate PAH levels could not be established since for the urban background and suburban-industrial sites the average concentrations of total PAHs in the PM2.5 fraction were very similar (1.085 and 1.151 ng m(-3), respectively), with benzo[b+k]fluoranthene and chrysene as the predominant compounds. Diagnostic ratios, used to identify PAH emission sources, pointed to traffic as the main source of particulate PAH at both locations. As expected, PAH levels at the rural site were significantly lower (0.408 ng m(-3) in the PM10 fraction) due to increasing distance from the emission sources. PAH seasonal variations at the urban background and suburban-industrial sites were the same as reported in many previous studies. Average winter to summer ratios for total PAHs were 4.4 and 4.9 for the urban background and industrial sites, in that order. This seasonal cycle could be partially explained by the higher temperature and solar radiation during summer enhancing PAH evaporation from the particulate phase and PAH photochemical degradation, respectively. The study of PAH distribution between the fine and coarse fraction at the urban site revealed that on average around 80% of total PAHs were associated with fine particles.     

Spatial and temporal distribution of polycyclic aromatic hydrocarbons (PAHs) in sediments of the Nansi Lake, China

Polycyclic aromatic hydrocarbons (PAHs) were measured in surface sediments and dated core sediments from the Nansi Lake of China to investigate the spatial and temporal distribution characteristics. The concentrations of 16 kinds priority PAH compounds were determined by GC-MS method. And ²¹⁰Pb isotope dating method was used to determine the chronological age of the sediment as well as the deposition rate. The results indicated that the total PAHs concentration ranges in surface and core sediment samples were 160 ~32,600 and 137 ~ 693 ng/g (dry wt.), respectively. The sediment rate and the average mass sedimentation were calculated to be 0.330 cm·year^???1 and 0.237 g·cm^???2·yr^???1 and the sediment time of the collected core sample ranged from 1899 to 2000. The peak of PAH concentrations came at recent years. The source analysis showed PAHs mainly came from the contamination of low temperature pyrogenic processes, such as coal combustion. The PAHs concentrations were lower than ERL and LEL values for most collected samples. However, in several surface sediment samples especially in estuary sites, the PAHs concentrations were not only higher than ERL and LEL values, but also higher than ERM values.     

Spatial and temporal trends of polycyclic aromatic hydrocarbons in wild mussels from the Cantabrian coast (N Spain) after the Prestige oil spill

Polycyclic aromatic hydrocarbon (PAH) levels were determined in tissues of wild mussels (Mytilus galloprovincialis) collected at 17 stations along the Cantabrian coast (N Spain), from Navia (Asturias) to Fuenterrabía (Basque Country), in order to assess the extent of the environmental impact caused by the Prestige oil spill (November 13, 2002). Six sampling campaigns were carried out in April, June and November in 2003 and 2004. The comparison of PAH data with those obtained earlier in 2000 showed a widespread pyrolytic and petrogenic contamination and allowed an estimation, for the first time, of the background pollution in the region and identification of the chronic hotspots. The spatial distribution found in the first samples after the oil spill revealed the eastern area as the most affected due to the continuous arrival of fuel slicks since early summer 2003. Several stations in this area showed increased total PAH concentrations of up to 15 times the pre-spill levels, which did not recover until April 2004, more than one year after the accident. Molecular parameters within the aliphatic and aromatic fractions were determined to assess the presence of Prestige oil in these samples.     

Environmental assessment of polycyclic aromatic hydrocarbons in the surface sediments of a remote region on the eastern coast,Taiwan

Surface sediment samples were collected in He-Ping Harbor and the nearby He-Ping Estuary from 2005 to 2006 to examine spatial and temporal variability in polycyclic aromatic hydrocarbon (PAH) concentrations. The sum of the 16 USEPA priority pollutant PAHs varied from 8 to 312 ng/g dry weight, which was relatively low compared to values obtained from other studies in the world. Regarding temporal changes in the PAH profile, total PAH concentrations in the wet season were lower than during the dry season in He-Ping Harbor. However, the concentration of PAHs exhibited no significant difference in the four seasons in the He-Ping Estuary. PAH concentrations in He-Ping Harbor were higher than those in the He-Ping Estuary. In comparison with sediment quality guidelines, PAH concentrations of sediments in this study were lower than those outlined in the criteria, which suggests no evident adverse biological effects due to PAHs around the He-Ping coast. Ratios of specific PAH compounds calculated to assess the possible sources of PAHs reflect that PAHs in He-Ping Harbor may mainly be from pyrogenic coal combustion.     

Characterization of PM10-bound polycyclic aromatic hydrocarbons in the ambient air of Spanish urban and rural areas

Urban areas constitute major pollution sources due to anthropogenic activities located in these areas. Among the legislated air pollutants, the particulate matter with an aerodynamic diameter less than or equal to 10 microns (PM10) and polycyclic aromatic hydrocarbons (PAH) are controlled under Directive 2008/50/EC and Directive 2004/107/EC, respectively due to their adverse health effects. A study was carried out at four urban and rural Spanish areas during the warm and cold seasons in 2008-2009 to quantify 19 PAH associated with the atmospheric PM10 by gas chromatography-mass spectrometry-mass spectrometry detection (GC-MS-MS) with the internal standard method. The particle-bound composition of the analysed PAH was 5 and 10 times greater in industrial and urban areas, respectively when compared to those measured in rural areas. The highest PAH concentrations during the cold period were possibly due to the additional contribution of domestic heating sources and meteorological conditions such as low temperature and solar irradiation. The use of molecular diagnostic ratios indicated that the possible, major PAH pollution sources in the most polluted areas were pyrogenic sources, mainly attributed to petroleum combustion sources (motor vehicle emissions and crude oil combustion). Petrogenic sources related to evaporative emissions also seemed to contribute in the most polluted area during the warm period. Those dates with high carcinogenic character according to the benzo(a)pyrene equivalent (BaP-eq) were also possibly attributed to petroleum combustion sources.     

Occurrence, source apportionment and toxicity assessment of polycyclic aromatic hydrocarbons in surface sediments of Chaohu, one of the most polluted lakes in China

In order to evaluate the effect of local anthropogenic activities on Chaohu Lake, one of the most eutrophicated lakes in China, surface sediments have been collected from the whole lake with 0.05 × 0.05 degree latitude/longitude resolution and in the estuaries of three main inflowing rivers. The concentrations of the 28 polycyclic aromatic hydrocarbons (PAHs) determined were in a range 82.4-13,000 ng g(-1) with an average value of 1670 ng g(-1) dry weight for total 28 PAHs (referred to as Σ(28)PAH). Amongst the 28 PAHs, 16 are listed as high priority PAHs by the USEPA and they were in the range of 60.8-10,200 ng g(-1) with an average value of 1230 ng g(-1) for the total of them (referred to as Σ(16)PAH); 7 are known as carcinogenic PAHs and their levels ranged from 34.2 to 6400 ng g(-1) with an average of 815 ng g(-1) in total (referred to as Σ(7)PAH). Chaohu Lake was considered significantly polluted by PAHs through the comparison with the PAH burdens in fresh-water lakes both in China and worldwide. Toxic units (TUs) evaluation showed some sampling locations possibly were over the median lethal level for benthic invertebrate. The highest PAH concentrations were found in sediments from the Nanfei River estuary, suggesting the major contributor of PAHs contamination to the lake. The PAHs with four and five rings were found to be dominant among the PAHs detected in all of the sediment samples, and perylene was the most abundant. Σ(16)PAH had a good correlation with those PAHs from pyrogenic sources, such as anthracene and phenanthrene, but a poor correlation with perylene. The results demonstrated that the environmental behavior of PAHs from pyrogenic sources is significantly different to that of perylene from diagenetic sources. The PAHs in sediments were mainly from traffic-related emission by qualitatively assessing with the diagnostic ratios of PAH isomers, and the ratios for low molecular weight PAHs were strongly altered during their transport.     

Determination of petroleum hydrocarbons and polycyclic aromatic hydrocarbons in sludge from wastewater treatment basins

Screening by gas chromatography with flame ionization detection and gas chromatography-mass spectrometry has been carried out on sludge extracts of wastewater treatment basins. Soxhlet extraction with trichlorotrifluoroethane was applied. The yields for petroleum hydrocarbons and PAH recovery were high, usually in excess of 90%. The proposed investigations permit a quick assessment of petroleum pollutants in the environment.     

A source study of atmospheric polycyclic aromatic hydrocarbons in Shenzhen, South China

Air pollution has become a serious problem in the Pearl River Delta, South China, particularly in winter due to the local micrometeorology. In this study, atmospheric polycyclic aromatic hydrocarbons (PAHs) were monitored weekly in Shenzhen during the winter of 2006. Results indicated that the detected PAHs were mainly of vapor phase compounds with phenanthrene dominant. The average vapor phase and particle phase PAHs concentration in Shenzhen was 101.3 and 26.7 ng m^???3, respectively. Meteorological conditions showed great effect on PAH concentrations. The higher PAHs concentrations observed during haze episode might result from the accumulation of pollutants under decreased boundary layer, slower wind speed, and long-term dryness conditions. The sources of PAHs in the air were estimated by principal component analysis in combination with diagnostic ratios. Vehicle exhaust was the major PAHs source in Shenzhen, accounting for 50.0% of the total PAHs emissions, whereas coal combustion and solid waste incineration contributed to 29.4% and 20.6% of the total PAHs concentration, respectively. The results clearly indicated that the increasing solid waste incinerators have become a new important PAHs source in this region.     

Source apportionment of polycyclic aromatic hydrocarbons in the Dahuofang Reservoir, Northeast China

Polycyclic aromatic hydrocarbons (PAHs) in 24 surface sediments from the Dahuofang Reservoir (DHF), the largest man-made lake in Northeast China, were measured. The results showed that the concentrations of 16 US EPA priority PAHs in the sediments ranged from 323 to 912 ng/g dry weight with a mean concentration of 592?±?139 ng/g. The PAH source contributions were estimated based on positive matrix factorization model. The coal combustion contributed to 31 % of the measured PAHs, followed by residential emissions (22 %), biomass burning (21 %), and traffic-related emissions (10 %). Pyrogenic sources contributed ～84 % of anthropogenic PAHs to the sediments, indicating that energy consumption release was a predominant contribution of PAH pollution in DHF. Compared with the results from the urban atmospheric PAHs in the region, there was a low contribution from traffic-related emissions in the sediments possibly due to the low mobility of the traffic-related derived 5+6-ring PAHs and their rapid deposition close to the urban area.     

Aliphatic and polycyclic aromatic hydrocarbons in sediments of Kaohsiung Harbour and adjacent coast, Taiwan

Surficial sediment samples collected from Kaohsiung Harbour and its nearby coast were analyzed for aliphatic hydrocarbons and parent polycyclic aromatic hydrocarbons (PAHs). According to our results, the average total concentrations of n-alkanes (n-C₁₂ to C₃₅) and aromatics (15 PAHs) were 4.33 µg g^–1 dry weight (ranged 0.46–22.60) and 0.59 µg g^–1 dry weight (ranged 0.09–1.75), respectively. The highest concentrations of aliphatic and aromatic hydrocarbons were recorded in stations near the estuaries of Qianzhen River and Love River, respectively. Aliphatic hydrocarbons in the samples indicate that there has been significant non-petrogenic, possibly terrestrial, contribution in the sediment of the open coast of Kaohsiung Harbour and that there has been dominant contribution from petrogenic sources in the sediment of the inner harbour. PAHs, detected in the samples, however, indicated a higher pyrolytic contribution in open-coast samples and a higher petrogenic contribution in the inner harbour. Overall, sediment concentrations of total alkanes in this study were comparable to those found in Victoria Harbour, Hong Kong and are higher than those found in Xiamen Harbour, China. Concentrations of total PAHs in inner Kaohsiung Harbour sediments were relatively lower than those found in Victoria Harbour, Hong Kong and Xiamen Harbour, China, but comparable to those found in Hsin-ta Harbour, Taiwan and Incheon Harbour, Korea. In comparison with several effect-based sediment quality guidelines, most PAH concentrations found in samples taken from inner harbour stations exceeded the Threshold Effect Level of Florida indicating a slight possibility of adverse effects.     

Identification of polycyclic aromatic hydrocarbons in unleaded petrol and diesel exhaust emission

Inhalation of emissions from petrol and diesel exhaust particulates is associated with potentially severe biological effects. In the present study, polycyclic aromatic hydrocarbons (PAHs) were identified from smokes released by the automobile exhaust from petrol and diesel. Intensive sampling of unleaded petrol and diesel exhaust were done by using 800-cm³ motor car and 3,455-cm³ vehicle, respectively. The particulate phase of exhaust was collected on Whatman filter paper. Particulate matters were extracted from filter paper by using Soxhlet. PAHs were identified from particulate matter by reverse phase high performance liquid chromatography using C₁₈ column. A total of 14 PAHs were identified in petrol and 13 in case of diesel sample after comparing to standard samples for PAH estimation. These inhalable PAHs released from diesel and petrol exhaust are known to possess mutagenic and carcinogenic activity, which may present a potential risk for the health of inhabitants.     

Characteristics and sources of atmospheric polycyclic aromatic hydrocarbons (PAHs) in Shanghai, China

A field campaign was conducted to measure and analyze 13 polycyclic aromatic hydrocarbons (PAHs) in six major zones in the city of Shanghai, P.R. China from August 2006 to April 2007. Ambient air samples were collected seasonally using passive air samplers, and gas chromatography–mass spectroscopy was used in this field campaign. The results showed that there was a sequence of 13 PAHs at Phen > FA > Pyr > Chr > Fl > An > BaA > BbFA > BghiP > IcdP > BkFA > BaP > DahA and the sum of these PAHs is 36.01 ± 10.85 ng/m³ in gas phase. FL, Phen, FA, Pyr, and Chr were the dominant PAHs in gas phase in the city. They contributed 90% of total PAHs in the gas phase. Proportion of measured PAHs with three, four, five, and six rings to total PAHs was 53%, 42%, 3%, and 2%, respectively. The highest concentration of ΣPAHs (the sum of 13 PAHs) occurred in the wintertime and the lowest was in the summer. This investigation suggested that traffic, wood combustion, and metal scrap burn emissions were dominant sources of the concentrations of PAHs in six city zones compared with coal burning and industry emissions. Further, the traffic emission sources of PAHs in the city were attributed mostly to gasoline-powered vehicles compared with diesel-powered vehicles. It was revealed that the seasonal changes in PAHs in the city depended on different source types. Metal scrap burn was found to be the major source of PAHs during the autumn, while the PAH levels in the atmosphere for winter and spring seasons were mainly influenced by wood and biomass combustion. Comparisons of PAHs among different city zones and with several other cities worldwide were also made and discussed.     

Distribution and sources of polycyclic aromatic hydrocarbons in Wuhan section of the Yangtze River, China

Polycyclic aromatic hydrocarbons (PAHs) are important organic contaminants with great significance for China, where coal burning is the main source of energy. In this study, concentrations, distribution between different phases, possible sources and eco-toxicological effect of PAHs of the Yangtze River were assessed. PAHs in water, suspended particulate matters (SPM) and sediment samples at seven main river sites, 23 tributary and lake sites of the Yangtze River at the Wuhan section were analyzed. The total concentrations of PAHs in the studied area ranged from 0.242 to 6.235 μg/l in waters and from 31 to 4,812 μg/kg in sediment. The average concentration of PAHs in SPM was 4,677 μg/kg, higher than that in sediment. Benzo(a)pyrene was detected only at two stations, but the concentrations were above drinking water standard. The PAHs level of the Yangtze River was similar to that of some other rivers in China but higher than some rivers in foreign countries. There existed a positive relationship between PAHs concentrations and the TOC contents in sediment. The ratio of specific PAHs indicated that PAHs mainly came from combustion process, such as coal and wood burning. PAHs may cause potential toxic effect but will not cause acute biological effects in sedimentary environment of the Wuhan section of the Yangtze River.     

Distribution of polycyclic aromatic hydrocarbons in marine sediments and their potential toxic effects

The presence of polycyclic aromatic hydrocarbons (PAHs) in samples of marine sediments from Paranagua Bay on the southern coast of Brazil was investigated. Paranagua Bay is the location of a major port, one of the busiest in Brazil. The region has a great potential for tourism and port-related industries and activities. Due to its characteristics as a venue for tourism, two major campaigns were planned: one 3 months before the summer (between December and February) and a second after the vacation season. Total concentration of PAHs in sediments ranged from 26.33 to 406.76 ng/g (in both campaigns). The highest values were found in sediments with higher organic carbon content. We found no substantial differences between the two campaigns, and the values are quite similar. Ternary diagrams show that points P5 and P6 were considered polluted, while others were classified as non-polluted. Molecular ratios indicate that the main sources of PAHs are petrogenic and the burning of fossil fuels. Sediment toxicity was assessed by the presence of PAHs in terms of benzo(a)pyrene (BaP) concentration. The toxicity of PAHs mixtures can be characterized more accurately by developing and establishing toxic equivalency factors (TEFs) for PAHs. Considering TEFs, the BaP_eq concentrations vary between 0.264 and 5.922 ng/g (considering both campaigns). Thus, two points are above the maximum level recommended (3 ng/g) by the Netherlands sediment quality guidelines. In fact, sites P5 and P6 apparently are exposed to a greater number of pollution sources, thus reflecting the higher concentration of PAHs compounds in sediments.     

Polychlorinated biphenyls, organochlorine pesticides and polycyclic aromatic hydrocarbons in a one-off global survey of bivalves

During the Danish Galathea 3 expedition, bivalve samples were collected at the Faroe Islands, Greenland, Ghana, South Africa, Australia, Solomon Islands, New Zealand, Chile, US Virgin Islands, Boston, Newfoundland and Shetland Islands and analysed for organochlorines and PAHs. Concentration differences of up to three orders of magnitude were observed, with the highest concentrations at Boston harbour (SPCB 338 ng g(-1) dw, ΣSPAH 5966 ng g(-1) dw) and the Sydney estuary (ΣSPCB 282 ng g(-1) dw, SPAH 1453 ng g(-1) dw). Local impacts were also found for the Greenland capital Nuuk in terms of PCB and PAH levels, while other Greenland samples came closest to representing PAH background levels. Several locations had undetectable organochlorine levels, including Hobart and Chile, which had the lowest SPAH concentrations (<200 ng g(-1) dw). It was possible to group the stations according to their pyrogenic/petrogenic influence using Principal Component Analyses, and indications of petroleum sources were found at Nuuk.     

Distribution and health-risk of polycyclic aromatic hydrocarbons in soils at a coking plant

Nineteen soil samples were collected in and around Songshan coking plant in Guangdong province of China and analyzed for eighteen polycyclic aromatic hydrocarbons (PAHs) by gas chromatography-mass spectrometry (GC-MS). The total concentration of PAHs ranged from 2.36 to 1146.39 mg kg(-1) dry weight, varying significantly among the sampling sites, most individual PAHs were correlated with each other. A cluster analysis was performed to examine the correlation of PAH distribution, five groups were observed with sample types in the coking plant. 2-3 ring PAHs were predominant in group I and II, while 4-5 ring PAHs showed great abundance in group III, IV and V, which contributed to the distance from the emission sources in the coking plant and the behaviors of particle-bound and gaseous PAHs. The ratios of Flu?:?(Flu + Pyr), BaA?:?(BaA + Chr), InP?:?(InP + BgP) and Ant?:?(Ant + Phen) ratios were 0.51-0.87, 0.16-0.89, 0.47-0.68 and 0.03-0.60, respectively. The total index of all studied soils was > 6, indicating that the source of the PAHs in coking plant soils were from the pyrolysis processes. Health risk assessments were carried out by dermal PAH exposure data to quantify cancer risk. The resultant lifetime exposure levels due to TEQ(BaP) desorbed onto skin for workers ranged from 2.25 × 10(-7) to 7.86 × 10(-5) mg kg(-1) per day, and the estimated cancer risks were between 8.45 × 10(-6) and 2.94 × 10(-3), indicating that the dermal exposures of PAHs to coking workers might be acceptable in most soil sites.