Atmospheric deposition of polycyclic aromatic hydrocarbons near New England coastal waters

Wet and dry deposition of polycyclic aromatic hydrocarbons (PAHs) was measured at Nahant, Massachusetts, a peninsula jutting into Massachusetts Bay and Wolf Neck, a peninsula jutting into Casco Bay, Maine. Wet deposition (rain and snow) was collected in a funnel which drains into a shielded, temperature controlled receiving bottle. Dry deposition of gaseous and particulate PAHs was collected onto an exposed water surface. PAHs were analyzed by solid phase extraction and gas chromatography-mass spectrometry. Sixteen PAH species were analyzed, ranging from acenaphthylene to coronene. The mean wet deposition rate of the sum of the 16 species is 720 ng m⁻² cm⁻¹ precipitation at Nahant, and 831 ng m⁻² cm⁻¹ precipitation at Wolf Neck. Wet deposition is attributed to regional PAH emitting sources. Storm patterns appear to bring somewhat higher wet deposition of PAHs to Wolf Neck than to Nahant. The mean dry deposition rate is 95 ng m⁻² h⁻¹ at Nahant and 9.3 ng m⁻² h⁻¹ at Wolf Neck. The large difference is attributed to the fact that Nahant is close to the urban-industrial metropolitan Boston area and Logan International Airport, whereas Wolf Neck has no major PAH-emitting sources nearby. Individual measurements have an error bracket of ±30%. The Chemical Mass Balance model was used to apportion the dry deposition to source categories. At Nahant, nine samples gave valid statistical attributes with a mean apportionment: jet exhaust 35%, gasoline fueled vehicles 32%, diesel fueled vehicles 17%, wood combustion 13%, others 3%. At Wolf Neck, six samples yielded a mean apportionment: jet exhaust 30%, gasoline vehicles 28%, diesel vehicles 18%, wood combustion 16%, others 8%. There is a considerable variation between the samples. The apportionment is greatly dependent on the quality and selection of the model inputs, i.e. source signatures, which for PAHs are questionable.     

Distribution and sources of polycyclic aromatic hydrocarbons in surface sediments of rivers and an estuary in Shanghai, China

Concentrations, spatial distribution and sources of 17 polycyclic aromatic hydrocarbons (PAHs) and methylnaphthalene were investigated in surface sediments of rivers and an estuary in Shanghai, China. Total PAH concentrations, excluding perylene, ranged from 107 to 1707 ng/g-dw. Sedimentary PAH concentrations of the Huangpu River were higher than those of the Yangtze Estuary. The concentration of the Suzhou River was close to the average concentration of the Huangpu River. PAHs source analysis suggested that, in the Yangtze Estuary, PAHs at locations far away from cities were mainly from petrogenic sources. At other locations, both petrogenic and pyrogenic inputs were significant. In the Huangpu and Suzhou Rivers, pyrogenic input outweighed other sources. The pyrogenic PAHs in the upper reaches of the Huangpu River were mainly from the incomplete combustion of grass, wood and coal, and those in the middle and lower reaches were from vehicle and vessel exhaust.     

空气中多环芳烃的研究进展

介绍了国内对大气中气态,颗粒态ＰＡＨｓ的研究概况,室内外空气中ＰＡＨｓ污染与城市交通间的相关性,ＰＡＨｓ总量代表物,硝基ＰＡＨｓ及人体接触ＰＡＨｓ的生物指标。     

Desorption of polycyclic aromatic hydrocarbons from field-contaminated soil to a two-dimensional hydrophobic surface before and after bioremediation

This study investigated environmental distributions and production mechanisms of chlorinated polycyclic aromatic hydrocarbons (Cl-PAHs) in the sediments from some tidal flats located in Asia. Cl-PAHs were found in sediments taken from Arao tidal flat, Kikuchigawa River and Shirakawa River. The range of ∑Cl-PAHs was from 25.5 to 483 pg g⁻¹ for Kikuchigawa River and Arao tidal flat, respectively.Concentrations of PAHs and Cl-PAHs showed no significant correlations (r = 0.134). This result suggests that the origins of these compounds differ. In the identified Cl-PAH isomers, the most abundant Cl-PAH isomer was 9,10-dichloroanthracene (9,10-di-Cl-ANT) in the three sites. In general, concentrations of Cl-ANTs in the coastal environment are about 3-5 orders of magnitude lower than those of anthracene (ANT). However, concentration ratios between Cl-ANTs and ANT (Cl-ANTs/ANT) in the sediments ranged from 4.1% to 24.6%. This result indicated that Cl-PAHs were not generated under industrial processes but the high concentration ratios have resulted from the contribution of photochemical production of Cl-ANTs in the sediments because ANT is known to have high photochemical reactivity.For examining this phenomenon, ANT adsorbed onto glass beads was irradiated with UV under the mimicked field conditions of tidal flats. As a result, it was noticed that, while chlorinated derivatives were negligible in a light-controlled group, production of 2-Cl-ANT, 9-Cl-ANT and 9,10-diCl-ANT on the irradiated surface were found in this study. These results suggest that photochemical reaction of PAHs can be a potential source of the occurrence of Cl-PAHs in the coastal environment.     

Size distribution of polycyclic aromatic hydrocarbons in a roadway tunnel in Lisbon, Portugal

Atmospheric aerosols of four aerodynamic size ranges were collected using high volume cascade impactors in an extremely busy roadway tunnel in Lisbon (Portugal). Dust deposited on the tunnel walls and guardrails was also collected. Average particle mass concentrations in the tunnel atmosphere were more than 30 times higher than in the outside urban background air, revealing its origins almost exclusively from fresh vehicle emissions. Most of the aerosol mass was concentrated in submicrometer fractions (65%), and polycyclic aromatic hydrocarbons (PAH) were even more concentrated in the finer particles with an average of 84% of total PAH present in sizes smaller than 0.49 μm. The most abundant PAH were methylated phenanthrenes, fluoranthene and pyrene. About 46% of the total PAH mass was attributed to lower molecular weight compounds (two and three rings), suggesting a strong influence of diesel vehicle emissions on the production of local particulate PAH. The application of diagnostic ratios confirmed the relevance of this source of PAH in the tunnel ambient air. Deposited dust presented PAH profiles similar to the coarser aerosol size range, in agreement with the predominant origin of coarser aerosol particles from soil dust resuspension and vehicle wear products.     

Determination of polycyclic aromatic hydrocarbons in urban street dust: implications for human health

The determination of sixteen polycyclic aromatic hydrocarbons in urban street dust has been done. Samples were collected from 12 sampling locations in a city centre location (Newcastle upon Tyne, north east England) and extracted using in situ pressurised fluid extraction followed by gas chromatography mass spectrometry. From the results it was possible to identify three groups, with respect to PAH concentration, with PAH contents ranging between 0.6-2.3 mg kg⁻¹, 15.6-22.5 mg kg⁻¹ and 36.1-46.0 mg kg⁻¹. The total PAH content of samples from these sampling sites has been compared to 22 urban locations around the world; comparable levels were found in these samples compared to the other cities around the world.The potential source of PAHs has been investigated by investigating the proportion of pyrogenic and petrogenic material in urban street dust using specific individual PAH ratios. The results indicate that the PAH content of urban street dust from the chosen sites are more likely to be due to pyrogenic sources i.e. vehicle exhaust emissions. The particle size fractions (<63 μm; 63-125 μm; 125-250 μm; 250-500 μm; 500-1000 μm; and 1000-2000 μm) of individual PAHs in three selected sampling sites was investigated. In two of the selected sites the PAH content was independent of particle size whereas in sampling site 10 elevated PAH levels are noted in the <63 μm size fraction. Sampling site 10 is located at the junction of three road tributaries which are used as major access points to the east of the city centre. Finally, the potential health risk for unintentional consumption of PAHs was assessed in terms of a mean daily intake (based on an ingestion rate of 100 mg d⁻¹). It was found that all 4-6 membered ring PAHs had concentrations in excess of the mean daily intake thereby reflecting a potential health risk, particularly in the smallest size particle fractions.     

紫外光(UV)光解油田采出水中多环芳烃

为了探讨紫外光光解人工模拟油田采出水中多环芳烃的降解效率,利用自制反应装置对油田采出水中多环芳烃(PAHs)的紫外光光解做了一个初步研究。研究结果证明,紫外光光解对油田采出水中的多环芳烃萘和芴有显著的降解能力。实验室的测试表明,与紫外UVA(365 nm)、UVB(308 nm)的光照相比,紫外UVC(254 nm)在光照60 min的条件下,2种多环芳烃各自的去除率都近似达到了99%。可见,在光解效力和暴露时间两方面,紫外UVC对采出水中萘和芴的去除具有相对稳定和比较高的效率。     

固相萃取-气相色谱/质谱法测定水中多环芳烃

建立了固相萃取-气相色谱／质谱联用测定水中多环芳烃(PAHs)的分析方法．优化了固相萃取条件。结果表明,固相萃取效率高、萃取时间短,采用MS的选择离子检测方式对实际水样中PAHs进行定性定量分析,平均回收率在80．4％～115％之间,相对标准偏差为7．03％～18．5％,方法的检出限在0．010～0．020μg／L之间。通过实际样品中PAHs的分析表明,该法快速,溶剂用量少,能满足痕量分析的要求。     

Anaerobic degradation of five polycyclic aromatic hydrocarbons from river sediment in Taiwan

This study investigated the anaerobic degradation of five polycyclic aromatic hydrocarbons (PAHs) from Erren River sediment in southern Taiwan. The degradation rates of PAH were in the order: acenaphthene > fluorene > phenanthrene > anthracene > pyrene. The degradation rate was enhanced when the five compounds were present simultaneously in river sediment. Comparison of the PAH degradation rates under three reducing conditions showed the following order: sulfate-reducing conditions > methanogenic conditions > nitrate-reducing conditions. The addition of electron donors (acetate, lactate and pyruvate) enhanced PAH degradation under methanogenic and sulfate-reducing conditions. However, the addition of acetate, lactate or pyruvate inhibited PAH degradation under nitrate-reducing conditions. The addition of heavy metals, nonylphenol and phthalate esters (PAEs) inhibited PAH degradation. Our results show that sulfate-reducing bacteria, methanogen and eubacteria are involved in the degradation of PAH; sulfate-reducing bacteria constitute a major microbial component in PAH degradation. Of the microorganism strains isolated from the sediment samples, we found that strain ER9 expressed the greatest biodegrading ability.     

Partitioning of polycyclic aromatic hydrocarbons to solid-sorbed nonionic surfactants

The partition of hydrophobic organic compounds (HOCs) into solid-sorbed surfactant has a crucial role in describing and predicting the distribution of HOCs in solid-water-surfactant systems. The experimental results of this study indicated that the partition coefficients of polycyclic aromatic hydrocarbons (PAHs) into the solid-sorbed surfactant (Ksm) increased with an increase in the sorption amount of surfactants onto solid and reached a stable maximum value (Km sm) at the sorption of surfactants in saturation state, at which the solid surface was completely covered with the surface micelle (or admicelle). The fitted Km sm values for PAHs with different surfactants were found to have a good linear relationship with the corresponding partition coefficient of PAHs to surfactant micelles in solution (Kmc), and then a model was developed to describe and predict the distribution of PAHs in solid-water-surfactant systems. These results are of practical interest for developing effective and safe surfactant-enhanced remediation technologies.     

Sources and distribution of polycyclic aromatic hydrocarbons in sediments from the Spanish northern continental shelf. Assessment of spatial and temporal trends

The distribution of polycyclic aromatic hydrocarbons was determined in surface sediments collected at 36 stations along the Spanish Northern continental shelf in March and September 2003, and February 2005. Concentrations of PAHs (Σ13 parent components) were in the range of 22-47528 μg/kg dw, the highest values corresponding to coastal urban-industrial hotspots and decreasing offshore. Sediment quality guidelines (SQGs) showed that concentrations of total PAHs were below the threshold effect level (TEC) in 27 stations (81%) and above in 7, two of which (Gijon and Bilbao) were above the probable effect concentration (PEC). The detailed study of diagnostic ratios suggested a rather uniform mixture of petrogenic and pyrolytic PAH sources along the continental shelf, with a slight decrease of the latter moving westwards and offshore. In order to assess the incidence of sediment sampling on the variability of the results, selected stations were also monitored in February and September 2004 and September 2005. The average field variance of the values obtained for each station was 31% that decreased to 23% when the values were normalized to TOC.     

Lead and polycyclic aromatic hydrocarbons (PAHs) in surface soil from day care centres in the city of Bergen, Norway

Surface soil (0-2cm) quality in 87 day care centres in the city of Bergen, Norway has been studied. Approximately 45% of the day care centres contained Pb and PAH values above recommended action levels. There are clear variations between different areas of the city. The old central part of the city hosts most of the contaminated day care centres. In suburban areas most of the day care centres have Pb and PAH concentrations below action levels. City fires, gas work emission, lead-based paint, and traffic are probably important anthropogenic contamination sources, together with uncontrolled transportation of soil from contaminated to clean areas. Geological or other natural sources are probably not an important contributor to the high levels of lead and PAH.     

Temperature-dependent sorption of polycyclic aromatic hydrocarbons on natural and treated sediments

In aqueous environment temperature is considered to play a significant role in the sorption process of polycyclic aromatic hydrocarbons (PAHs) and its influence on the sorption equilibrium is indicative of sorption energies and mechanisms. In this study, sorptions of five PAHs on three heterogeneous sorbents including one river sediment (YHR), one estuary sediment (YRD) and one treated sediment with organic matter removed (IM) were carried out at a range of temperature from 5 °C to 35 °C. Stronger sorptions were observed at lower temperatures, with the equilibrium sorption coefficient K_d increasing 2-5 times as the temperature decreases 30 °C. The increase of K_d value was attributed primarily to the change of PAH water solubility, which predicted 40-75% of the increase of K_d in the sorption process. To provide insight into the sorption mechanism, enthalpy change (ΔH_S) for the sorption process was calculated and the values were observed to be negative for all of the interactions, suggesting that the exothermal sorption of PAHs inversely dependents on temperature. Based on the values of ΔH_S, van der Waals forces were inferred as the main sorption mechanism for the PAHs, especially on the YHR sediment which contained more organic matter. For sorption of larger size PAHs on the sorbents with low organic matter, specific interactions were deduced to contribute to the overall sorption.     

Characterization of extractable and non-extractable polycyclic aromatic hydrocarbons in soils and sediments from the Pearl River Delta, China

Formation of bound residues of pollutants in soils and sediments is an important process to control the fate of pollutants in the environment. The most of bound residue is not solvent extractable. In this paper, we measured both extractable and non-extractable polycyclic aromatic hydrocarbons (PAHs) in different organic matter fractions of samples from the Pearl River Delta, China. Non-extractable PAHs concentration was 234.45-1424.57 μg/kg and accounted for 33.78-57.44% of total PAHs. 2-3 Ring PAHs were the dominant species and differed in concentration substantially between the samples. The atomic ratio of PAHs over organic-C in the fractions ordered as solvent soluble organic matter > humin > humic acids, matching the content of aliphatic moieties in the fractions of organic matter. The ratio of extractable and non-extractable PAHs may relate to the aging process of PAHs in soil and sediment.     

A comparative study on the uptake of polycyclic aromatic hydrocarbons by Anodonta californiensis

Uptake of polycyclic aromatic hydrocarbons (PAHs) by the freshwater bivalve mollusc Anodonta californiensis was examined in the presence and absence of surfactant in order to gain further insight into mixture toxicity and to predict whether certain mixtures have negative and/or positive effects on aquatic organisms. In the presence of surfactant, the uptake of anthracene or chrysene was higher than that of naphthalene, given the same concentration in the solution. In the absence of surfactant, the trend was similar, but the uptakes were increased by approximately 100% compared to those in the presence of surfactant. On the uptake of naphthalene, the presence of anthracene showed only minor influence. The uptake of anthracene was affected by both naphthalene and chrysene. The uptake of chrysene was influenced by neither naphthalene nor anthracene. There was no observable displacement of divalent cations from the surface of the gill membrane by any of the PAHs studied.     

Variations in concentrations and compositions of polycyclic aromatic hydrocarbons (PAHs) in coals related to the coal rank and origin

The release of unburnt coal particles and associated polycyclic aromatic hydrocarbons (PAHs) may cause adverse impacts on the environment. This study assessed variations in the concentration and composition of PAHs in a set of fifty coal samples from eleven coal basins worldwide. The maximum PAH concentrations at high volatile bituminous rank were recorded in samples from a single basin. Considering the entire sample set, the highest PAH concentrations were in fact found outside of this rank range, suggesting that the maceral composition and thus the coal’s origin also influenced PAH concentrations. The examination of the PAH compositions revealed that alkylated 2-3 ring PAHs remain dominant compounds irrespective of coal rank or origin. Multivariate analysis based on PAH and maceral content, bulk and maturity parameters allowed the recognition of seven groups with different rank and origin within the coal sample set.     

Relative proportions of polycyclic aromatic hydrocarbons differ between accumulation bioassays and chemical methods to predict bioavailability

Chemical methods to predict the bioavailable fraction of organic contaminants are usually validated in the literature by comparison with established bioassays. A soil spiked with polycyclic aromatic hydrocarbons (PAHs) was aged over six months and subjected to butanol, cyclodextrin and tenax extractions as well as an exhaustive extraction to determine total PAH concentrations at several time points. Earthworm (Eisenia fetida) and rye grass root (Lolium multiflorum) accumulation bioassays were conducted in parallel. Butanol extractions gave the best relationship with earthworm accumulation (r² ≤ 0.54, p ≤ 0.01); cyclodextrin, butanol and acetone-hexane extractions all gave good predictions of accumulation in rye grass roots (r² ≤ 0.86, p ≤ 0.01). However, the profile of the PAHs extracted by the different chemical methods was significantly different (p < 0.01) to that accumulated in the organisms. Biota accumulated a higher proportion of the heavier 4-ringed PAHs. It is concluded that bioaccumulation is a complex process that cannot be predicted by measuring the bioavailable fraction alone.     

Anthropogenic input of polycyclic aromatic hydrocarbons into five lakes in Western China

The temporal distribution of polycyclic aromatic hydrocarbons (PAHs) was examined in dated sediments from five lakes in Western China. The surficial concentrations of seven carcinogenic PAHs (BaA, Chyr, BbF, BkF, BaP, DBA and INP, hereafter denoted as PAH₇) were highly site-specific. The ΣPAH₇ concentrations generally increased from the deep layers to surface sediments. The temporal trends of ΣPAH₇ concentrations were clearly different from those reported in developed countries. From 1950s to 1980s, which PAHs started to decrease in developed countries, is the right period that PAHs started to increase rapidly in Western China. The fluxes and mass inventories suggest that the PAH₇ input over the past three decades was much more rapidly than it was before the 1980s. Source identification indicates that the PAHs were primarily from biomass burning and domestic coal combustion, and increasing vehicular and/or industrial coal combustion emission was also found.     

北方某城市饮用水中多环芳烃的来源及其在水处理过程中的行为研究

采用固相萃取(SPE)样品富集前处理技术和气相色谱/质联联用(GC/MS)分析方法,对北方某工业城市给水系统中的多环芳烃类化合物的含量水平进行了研究.结果表明,该城市多环芳烃污染水平较高,但总浓度均未超过城市供水水质标准(CJ/T206-2005)中限值(2μg/L).近郊水库由于受到燃料燃烧产生的多环芳烃的污染,成为该市饮用水中多环芳烃污染的主要来源.传统的混凝-砂滤工艺对多环芳烃有较好的去除效果,总去除率可达55.9%.     

Occurrence of polycyclic aromatic hydrocarbons in surface sediments of a highly urbanized river system with special reference to energy consumption patterns

Sediment samples collected from downstream of the Dongjiang River, a highly urbanized river network within the Pearl River Delta of South China, were analyzed for 28 polycyclic aromatic hydrocarbons (PAHs). Total concentrations of 28 PAHs, 16 priority PAHs designated by the United States Environmental Protection Agency (USEPA) and the seven carcinogenic PAHs classified by the USEPA ranged from 480 to 4600, 100 to 3400 and 10 to 1700 ng/g dry weight, respectively. Principal component analysis-based stepwise multivariate linear regression showed that sediment PAHs were predominantly derived from coal combustion, refined fossil fuel combustion and oil spills, accounting for 37%, 32% and 23%, respectively, of the total loading. The levels of sediment PAHs remained steady from 2002 to 2008, during which fossil fuel consumption had doubled, probably reflecting efforts to control PAH emissions from fossil fuel combustion. Finally, use of natural gas and liquefied petroleum gas in automobiles should be encouraged to improve environmental quality.