Spatial distribution and seasonal variation of atmospheric bulk deposition of polycyclic aromatic hydrocarbons in Beijing-Tianjin region, North China

Bulk deposition samples were collected in remote, rural village and urban areas of Beijing-Tianjin region, North China in spring, summer, fall and winter from 2007 to 2008. The annually averaged PAHs concentration and deposition flux were 11.81 ± 4.61 μg/g and 5.2 ± 3.89 μg/m²/day respectively. PHE and FLA had the highest deposition flux, accounting for 35.3% and 20.7% of total deposition flux, respectively. More exposure risk from deposition existed in the fall for the local inhabitants. In addition, the PAHs deposition flux in rural villages (3.91 μg/m²/day) and urban areas (8.28 μg/m²/day) was 3.8 and 9.1 times higher than in background area (0.82 μg/m²/day), respectively. This spatial variation of deposition fluxes of PAHs was related to the PAHs emission sources, local population density and air concentration of PAHs, and the PAHs emission sources alone can explain 36%, 49%, 21% and 30% of the spatial variation in spring, summer, fall and winter, respectively.     

Spatial and seasonal variations of polycyclic aromatic hydrocarbons in Haihe Plain, China

A dynamic fugacity model was developed to simulate the spatial and seasonal variations of PAHs in Haihe Plain, China. The calculated and measured concentrations exhibited good consistency in magnitude with deviations within a factor of 4 in air and 2 in soil. The spatial distributions of PAHs in air were mainly controlled by emission while the seasonal variations were dominated by emission and gas-particle partition. In soil, the spatial distributions of PAHs were controlled by the soil organic carbon content while the seasonal variations were insignificant. The severest soil contamination was observed in Shanxi and followed by the southwest of Hebei province. Transfer fluxes of total PAHs between air and soil were calculated. The spatial distribution of air-to-soil flux was closely related to the landcover while the soil-to-air flux changed with soil organic matter content. Monte Carlo simulation was done to evaluate the uncertainty of the estimated results in air.     

Sources and patterns of polycyclic aromatic hydrocarbons pollution in kitchen air,China

Twelve polycyclic aromatic hydrocarbons, multi-ringed compounds known to be carcinogenic in air of six domestic kitchens and four commercial kitchens of China were measured in 1999-2000. The mean concentration of total PAHs in commercial kitchens was 17 microg/m3, consisting mainly of 3- and 4-ring PAHs, and 7.6 microg/m3 in domestic kitchens, where 2- and 3-ring PAHs were predominant, especially naphthalene. The BaP levels in domestic kitchens were 0.0061-0.024 microg/m3 and 0.15- 0.44 microg/m3 in commercial kitchens. Conventional Chinese cooking methods were responsible for such heavy PAHs pollution. The comparative study for PAH levels in air during three different cooking practices: boiling, broiling and frying were conducted. It was found that boiling produced the least levels of PAHs. For fish, a low-fat food, frying it produced a larger amount of PAHs compared to broiling practice, except pyrene and anthracene. In commercial kitchens, PAHs came from two sources, cooking practice and oil-fumes, however the cooking practice had a more predominant contribution to PAHs in commercial kitchen air. In domestic kitchens, except for cooking practice and oil-fumes, there were other PAHs sources, such as smoking and other human activities in the domestic houses, where 3-4 ring PAHs mainly came from cooking practice. Naphthalene (NA, 2-ring PAHs) was the most predominant kind, mostly resulting from the evaporation of mothball containing a large quantity of NA, used to prevent clothes against moth. A fingerprint of oil-fumes was the abundance of 3-ring PAHs. Heating at the same temperature, the PAHs concentrations in different oil-fumes were lard > soybean oil > rape-seed oil. An increase in cooking temperature increased the levels of PAHs, especially acenaphthene.     

Implications for long-range atmospheric transport of polycyclic aromatic hydrocarbons in Lhasa, China

The Tibetan Plateau is suggested to be an important indicator region to study the global long-range atmospheric transport of persistent organic pollutants. In this study, atmospheric polycyclic aromatic hydrocarbons (PAHs) were studied in Lhasa City in the Tibetan Plateau, China. Air samples in gas and particle phases were concurrently collected by a modified high-volume air sampler from 5 August 2008 to 13 July 2009. The concentration of ∑₁₆PAHs ranged from 18 to 160 ng?m^?3 (with a geometric mean of 68 ng?m^?3). The most abundant PAHs were phenanthrene and benzo(b)fluoranthene in gas and particle phases, respectively. Compared with other two similar studies in Beijing and Harbin, different temporal trends were found between gas and particle phases PAHs in Lhasa. The influences of meteorological parameters (ambient temperature and relative humidity) and air masses from China, India, Southeast Asia, and West Asia were the two important reasons for explaining the difference, which was confirmed by the 5-day backward trajectories. This is the first comprehensive study to provide the evidence for the different influences of long-range atmospheric transport on gas and particle phases PAHs pollution in the Tibetan Plateau.     

Partitioning and source diagnostics of polycyclic aromatic hydrocarbons in rivers in Tianjin, China

Water, suspended particulate matter (SPM), and sediment samples were collected from ten rivers in Tianjin and analyzed for 16 polycyclic aromatic hydrocarbons (PAHs), dissolved organic carbon (DOC), particulate organic carbon (POC) in SPM and total organic carbon (TOC) in sediment. The behavior and fate of PAHs influenced by these parameters were examined. Generally, organic carbon was the primary factor controlling the behavior of the 16 PAH species. Partitioning of PAHs between SPM and water phase was studied, and K(OC) for some PAH species were found to be significantly higher than the predicted values. The source of PAHs contamination was diagnosed by using PAH isomer ratios. Coal combustion was identified to be a long-term and prevailing contamination source for sediment, while sewage/wastewater source could reasonably explain a short-term PAHs contamination of SPM.     

Seasonal variation of polycyclic aromatic hydrocarbons (PAHs) emissions in China

A regression model based on the provincial energy consumption data was developed to calculate the monthly proportions of residential energy consumption compared to the total year volume. This model was also validated by comparing with some survey and statistical data. With this model, a PAHs emission inventory with seasonal variation was developed. The seasonal variations of different sources in different regions of China and the spatial distribution of the major sources in different seasons were also achieved. The PAHs emissions were larger in the winter than in the summer, with a difference of about 1.3-folds between the months with the largest and the smallest emissions. Residential solid fuel combustion dominated the pattern of seasonal variation with the winter-time emissions as much as 1.6 times as that in the summer, while the emissions from wild fires and open fire straw burning was mainly concentrated during the spring and summer.     

Seasonal variations and source apportionment of atmospheric PM2.5-bound polycyclic aromatic hydrocarbons in a mixed multi-function area of Hangzhou,China

Environmental Science and Pollution Research - To reveal the seasonal variations and sources of PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) during haze and non-haze episodes, daily PM2.5...     

Characteristics and sources of environmentally persistent free radicals in PM2.5 in Dalian,Northeast China: correlation with polycyclic aromatic hydrocarbons

Environmental Science and Pollution Research - Environmentally persistent free radicals (EPFRs) are an emerging class of environmental hazardous contaminants that extensively, stably exist in...     

Ice phase as an important factor on the seasonal variation of polycyclic aromatic hydrocarbons in the Tumen River,Northeastern of China

Background, aim and scope  

The climatic characteristic is a major parameter affecting on the distribution variation of organic pollutants such as polycyclic aromatic hydrocarbons (PAHs). The Tumen River is located in Northeastern of China. The winter era lasts for more than 5 months in a year, and the river water was frozen and covered by ice phase. Coal combustion is an essential heating source in the Tumen River Basin. The objective of this research is to study ice phase effect on the seasonal variation of PAHs in the Tumen River environment.     

Distribution and sources of polycyclic aromatic hydrocarbons from urban to rural soils: a case study in Dalian, China

To estimate the distribution and sources of soil polycyclic aromatic hydrocarbons (PAHs) in metropolitan and adjacent areas, soil samples were collected from urban, suburban and rural locations of Dalian, China, and concentrations of 14 PAHs were determined. The spatial PAH profiles were site-specific and determined by the sources close to the sampling sites. PAH concentrations decreased significantly along the urban-suburban-rural transect. The gradient implied that the fractionation effect influenced PAH distribution. Bivariate plots of selected diagnostic ratios showed general trends of co-variation and allowed to distinguish samples taken from different areas. An improved method, factor analysis (FA) with nonnegative constrains, was used to determine the primary sources and contributions of PAHs in soils. The FA model showed traffic average (74%) and coal related residential emission (26%) were two primary sources to Dalian soils. In addition, the FA model provided reasonable explanations for PAH contributions in soils from different sites. The results suggest that FA with nonnegative constraints is a promising tool for source apportionment of PAHs in soils.     

Spatial and seasonal variation and sources of deposition fluxes of polycyclic aromatic hydrocarbons (PAHs) in Shanghai

Environmental Science and Pollution Research - Spatial and temporal variations of polycyclic aromatic hydrocarbons (PAHs) deposition fluxes and sources may significantly facilitate risk evaluation...     

Oxygenated polycyclic aromatic hydrocarbons in atmospheric particulate matter: Molecular characterization and occurrence

Particulate matter (PM) has become a major research issue receiving increasing attention because of its significant negative impact on human health. There are main indicators that next to the morphological characteristics of the particle, also the chemical composition plays an important role in the adverse health effects of PM. In this context, the rather polar organic fraction of PM is expected to play a major role, and advanced analytical techniques are developed to improve the knowledge on the molecular composition of this fraction. One component class that deserves major attention consists of the oxygenated polycyclic aromatic hydrocarbons (PAHs). Those compounds are considered to be among the key compounds in PM toxicity. This paper presents a comprehensive review focusing on the analysis, fate and behavior of oxygenated PAHs in the atmosphere. The first part of the paper briefly introduces (i) the main sources and atmospheric pathways of oxygenated PAHs, (ii) available physical–chemical properties and (iii) their health effects. The second and main part of this paper gives a thorough discussion on the entire analytical sequence necessary to identify and quantify oxygenated PAHs on atmospheric PM. Special attention is given to critical parameters and innovations related to (i) sampling, (ii) sample preparation including both extraction and clean-up, and (iii) separation and detection. Third, the state-of-the-art knowledge about the atmospheric occurrence of oxygenated PAHs is discussed, including an extended overview of reported concentrations presented as a function of sampling season and geographical location. A clear seasonal effect is observed with the median of the oxygenated PAHs concentrations during winter being a factor of 3–4 higher than during summer. However, the oxygenated PAH/parent PAH ratio is about 20 times higher during summer, indicating the importance of photochemical activity in the atmosphere.     

Biomonitoring seasonal variation of urban air polycyclic aromatic hydrocarbons (PAHs) using Ficus benghalensis leaves

Temporal and seasonal variations of polycyclic aromatic hydrocarbons (PAHs) concentrations in leaves of Ficus benghalensis were investigated in Varanasi city (India). Leaf samples were collected from six sites from urban area of Varanasi and from a control site. PAH extraction was done by sonication in dichloromethane-acetone and quantification by GC-MS. In January total leaf PAHs concentrations at all the urban sites were twice higher as compared to other season's viz. summer and rainy. In contrast, at the control site leaf PAHs concentrations showed lower values than urban sites. The maximum concentrations of total PAHs in winter were due to the medium molecular weight PAHs which increases with respect to both low and high molecular weight PAHs. The temporal variation of medium molecular weight PAHs was similar both at the urban and remote sites. These results support biomonitoring ability of Ficus benghalensis leaves to temporal variations in PAHs contamination.     

Seasonal variation of polycyclic aromatic hydrocarbons (PAHs) in Pearl River Delta region,China

A level IV fugacity model was applied to simulate the seasonal variation of polycyclic aromatic hydrocarbons (PAHs) in various bulk media in Pearl River Delta (PRD), China. The predictions were validated against monthly observed concentrations of gaseous and particulate phase PAHs in air and annual mean concentrations of all other bulk media. The uncertainty of the predictions was evaluated using Monte Carlo simulation. The influential parameters were identified using sensitivity analysis on both media concentrations and seasonal variations. The predicted concentrations and the patterns of seasonal variation generally agreed with the field observations. Concentrations of gaseous phase PAHs in air increased in the summer and decreased in the winter while concentrations of particulate phase PAHs in summer were lower than those in the winter. The relative variations of PAHs in the other bulk media were not as profound as those in air and the variation patterns were chemical compound dependent. Temperature and precipitation were the most important parameters leading to the seasonalities of PAH concentrations. Other key parameters included dry precipitation rate, advective water flow from upstream, and solid fractions in air and water.     

Mobile sources of atmospheric polycyclic aromatic hydrocarbons in a roadway tunnel

Amounts of polycyclic aromatic hydrocarbons (PAHs) and oxygenated polycyclic aromatic hydrocarbons (oxy-PAHs) in samples collected from the air, from the dust on a guardrail, and from the soils on a tunnel roadway at five sampling sites in a regular roadway tunnel were chemically analyzed in order to determine their sources. Among the 23 PAHs found in the air samples, pyrene was found in the highest concentration (43±7.2 ng/m³), followed by fluoranthene (26±4.3 ng/m³). Among 20 oxy-PAHs found in the air samples, anthraquinone was found in the greatest amount (56±3.9 ng/m³). The average concentration of the major PAHs found in the guardrail dust samples were 6.9±0.77 μg/g for pyrene, 5.5±0.76 μg/g for fluoranthene, and 2.6±0.30 μg/g for phenanthrene. The average concentration of the major oxy-PAHs found in the guardrail dust samples were 9.2±3.5 μg/g for anthraquinone and 1.4±0.50 μg/g for 2-methylanthraquinone. The average concentration of the major PAHs found in the soil samples were 1.1±0.31 μg/g for fluoranthene, 0.92±0.21 μg/g for pyrene, and 0.72±0.16 μg/g for phenanthrene. The average concentration of the major oxy-PAHs found in the soil samples were 1.2±0.88 μg/g for anthraquinone, 0.18±0.04 μg/g for 4-biphenylcarboxaldehyde, and 0.13±0.08 μg/g for 2-methylanthraquinone. The BeP ratios calculated from the results suggest that most PAHs found in the samples collected from the roadway tunnel were from automobile exhaust gases.     

Contamination of rivers in Tianjin, China by polycyclic aromatic hydrocarbons

Tianjin urban/industrial complex is highly polluted by some persistent organic pollutants. In this study, the levels of 16 priority polycyclic aromatic hydrocarbons (PAHs) were tested in sediment, water, and suspended particulate matter (SPM) samples in 10 rivers in Tianjin. The total concentration of 16 PAHs varied from 0.787 to 1943 microg/g dry weight in sediment, from 45.81 to 1272 ng/L in water, and from 0.938 to 64.2 microg/g dry weight in SPM. The levels of PAHs in these media are high in comparison with values reported from other river and marine systems. Variability of total concentrations of PAHs in sediment, water, and SPM from nine different rivers is consistent with each other. No obvious trends of total PAHs concentration variations were found between upstream and downstream sediment, water, and SPM samples for most rivers, which indicate local inputs and disturbances along these rivers. The spatial distributions of three-phase PAHs are very similar to each other, and they are also similar to those found in topsoil. However, their chemical profiles are significantly different from that of topsoil. The change of profiles is consistent with the different aqueous transport capability of 16 PAHs. Low molecular weight PAHs predomination suggests a relatively recent local source and coal combustion source of PAHs in the study area.     

Chlorinated polycyclic aromatic hydrocarbons in surface sediment from Maowei Sea,Guangxi, China: occurrence,distribution, and source apportionment

Environmental Science and Pollution Research - Chlorinated polycyclic aromatic hydrocarbons (ClPAHs) with three to five aromatic rings have been documented to ubiquitously occur in environmental...     

Modelling the atmospheric fate and seasonality of polycyclic aromatic hydrocarbons in the UK

This paper presents the results from an exercise in atmospheric contaminant fate modelling, which had three main objectives: (1) to investigate the balance between estimated national atmospheric emissions of six selected PAHs and observed ambient measurements for the UK, as a means of testing the current emission estimates; (2) to investigate the potential influence of seasonally dependent environmental fate processes on the observed seasonality of air concentrations; and (3) after undertaking the first two objectives, to make inferences about the likely magnitude of seasonal differences in sources. When addressing objective 1 with annually averaged emissions data, it appeared that the UK PAH atmospheric emissions inventory was reasonably reliable for fluorene, fluoranthene, pyrene, benzo[a]pyrene and benzo[ghi]perylene--but not so for phenanthrene. However, more detailed analysis of the seasonality in environmental processes which may influence ambient levels, showed that the directions and/or magnitudes of the predicted seasonality did not coincide with field observations. This indicates either that our understanding of the environmental fate and behaviour of PAHs is still limited, and/or that there are uncertainties in the emissions inventories. It is suggested that better quantification of PAH sources is needed. For 3- and 4-ringed compounds, this should focus on those sources which increase with temperature, such as volatilisation from soil, water, vegetation and urban surfaces, and possible microbially-mediated formation mechanisms. The study also suggests that the contributions of inefficient, diffusive combustion processes (e.g. domestic coal/wood burning) may be underestimated as a source of the toxicologically significant higher molecular weight species in the winter. It is concluded that many signatory countries to the UNECE POPs protocol (which requires them to reduce national PAH emissions to 1990 levels) will experience difficulties in demonstrating compliance, because source inventories for 1990 and contemporary situations are clearly subject to major uncertainties.     

乌鲁木齐市大气可吸入颗粒物中多环芳烃的污染特征及来源解析

在乌鲁木齐市南、北设置2个采样点,从2011年3-12月采集可吸入颗粒物(PM2.5、PM2.5-10)样品,分析了美国环境保护署优控的13种多环芳烃(PAHs)的浓度,采用比值法、主成分分析法和多元线性回归法对乌鲁木齐市大气PM2.5、PM2.5-10中PAHs的来源进行了分析。结果表明,科学院站PM2.5中13种PAHs的总质量浓度平均值为247.2ng/m3,变动范围为1.14~2 113.33ng/m3;新大站PAHs的总质量浓度平均值为240.84ng/m3,变动范围为4.96~1 359.41ng/m3。而科学院站PM2.5-10中13种PAHs的总质量浓度平均值为57.78ng/m3,变动范围为1.18~519.87ng/m3;新大站的总质量浓度平均值为49.18ng/m3,变动范围为1.38~412.52ng/m3。比值法分析结果表明,所采集样品的2/3来自煤和生物质的燃烧排放;主成分分析法和多元线性回归分析法结果表明,采暖期汽油和煤源对PM2.5中总PAHs的贡献率为46%,而非采暖期混合源的贡献率高达85%。采暖期汽油和柴油源对PM2.5-10中总PAHs的贡献率为66%,而非采暖期混合源的贡献率为78%。     

Characterization of atmospheric polycyclic aromatic hydrocarbons in a mixed-use urban community in Paterson, NJ: concentrations and sources

Exposure to ambient polycyclic aromatic hydrocarbons (PAHs) is a potential health concern for communities because many PAHs are known to be mutagenic and carcinogenic. However, information on ambient concentrations of PAHs in communities is very limited. During the Urban Community Air Toxics Monitoring Project, Paterson City, NJ, PAH concentrations in ambient air PM10 (particulate matter < or = 10 microm in aerodynamic diameter) were measured from November 2005 through December 2006 in Paterson, a mixed-use urban community located in Passaic County, NJ. Three locations dominated by industrial, commercial, and mobile sources were chosen as monitoring sites. The comparison background site was located in Chester, NJ, which is approximately 58 km west/southwest of Paterson. The concentrations of all of the individual PAHs at all three Paterson sites were found to be significantly higher than those at the background site (P < 0.05). The PAH profiles obtained from the three sites with different land-use patterns showed that the contributions of heavier PAHs (molecular weight > 202) to the total PAHs were significantly higher at the industrial site than those at the commercial and mobile sites. Analysis of the diagnostic ratios between PAH isomers suggested that the diesel-powered vehicles were the major PAH sources in the Paterson area throughout the year. The operation of industrial facilities and other combustion sources also partially contributed to PAH air pollution in Paterson. The correlation of individual PAH, total PAH, and the correlation of total PAHs with other air co-pollutants (copper, iron, manganese, lead, zinc, elemental carbon, and organic carbon) within and between the sampling sites supported the conclusions obtained from the diagnostic ratio analysis.