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1.
Polycyclic aromatic hydrocarbons (PAHs) in PM2.5 and cloud/fog water samples were collected at Mount Taishan in an autumn–winter period, and were analyzed by GS-MS. Higher molecular weight PAHs (4–6 rings) predominated in PM2.5 samples, whereas lighter PAH compounds contributed 61.71% of the total PAH concentration in cloud/fog samples. Particles tended to contain more PAHs and have a more intensive influence on the atmospheric environment on colder days. During cloud/fog events, the scavenging ratio based on PAHs associated with particles was estimated to be about 13.45%. PAHs in PM2.5 samples had a significant positive relationship with CO and SO2, suggesting that PAHs, SO2, and CO may originated from the same sources, such as residential coal combustion activities. Diagnostic ratio analysis and factor analysis indicated that the sources of PAHs were mainly from coal combustion during this period.  相似文献   

2.
Soil derived sources of polycyclic aromatic hydrocarbons (PAHs) in the region of Dalian, China were investigated using positive matrix factorization (PMF). Three factors were separated based on PMF for the statistical investigation of the datasets both in summer and winter. These factors were dominated by the pattern of single sources or groups of similar sources, showing seasonal and regional variations. The main sources of PAHs in Dalian soil in summer were the emissions from coal combustion average (46%), diesel engine (30%), and gasoline engine (24%). In winter, the main sources were the emissions from coal-fired boiler (72%), traffic average (20%), and gasoline engine (8%). These factors with strong seasonality indicated that coal combustion in winter and traffic exhaust in summer dominated the sources of PAHs in soil. These results suggested that PMF model was a proper approach to identify the sources of PAHs in soil.  相似文献   

3.
The assessment of polycyclic aromatic hydrocarbons (PAHs) contamination in surface sediments from the Yangtze estuary which is a representative area affected by anthropogenic activity (rapid industrialization, high-population density, and construction of dams upstream) in the world was systematically conducted. Fifty-one samples were analyzed by high-performance liquid chromatography (HPLC). The ??PAHs in all sediments varied from 76.9 to 2,936.8?ng?g?1. Compared with other estuaries in the world, the PAH levels in the Yangtze estuary are low to moderate. Phenanthrene, acenaphthylene, fluoranthene, and pyrene were relatively abundant. The ??PAH levels and composition varied obviously in different estuarine zones due to different sources. The highest ??PAHs concentration was observed in the nearshore of Chongming Island. The PAH composition showed that four to six ring PAHs were mainly found in the nearshore areas, while two to three ring PAHs were in the farther shore zones. The PAHs in the Yangtze estuary were derived primarily from combustion sources. A mixture of petroleum combustion and biomass combustion mainly from coal combustion and vehicle emission was the main source of PAHs from the nearshore areas, while the spill, volatilization, or combustion of petroleum from shipping process and shoreside discharge were important for PAHs in the farther shore areas. The result of potential ecotoxicological risk assessment based on sediment quality guidelines indicated low PAH ecological risk in the Yangtze estuary. The study could provide foundation for the protection of water quality of the Yangtze estuary by inducing main sources input.  相似文献   

4.
The spatial distribution, composition, and sources of polycyclic aromatic hydrocarbons (PAHs) in sediments and suspended particulate matter (SPM) from the Pearl River Estuary and adjacent coastal areas were examined. Total PAH concentrations varied from 189 to 637 ng/g in sediments and 422 to 1,850 ng/g in SPM. PAHs were dominated by 5,6-ring compounds in sediments and by 2,3-ring compounds in SPM samples. Assessment of PAH sources suggested that biomass and coal combustion is the major PAH source to the outer part of the estuary sediments and that petroleum combustion is the major PAH source to the inner part of estuary sediments. As for SPM samples, PAH isomer pair ratios indicated multiple (petroleum, petroleum combustion, and biomass and coal combustion) PAH sources, and significant temporal variations could exist for the sources of water column PAHs in the study area. The distribution of perylene in SPM samples indicated that the river was the dominant source of perylene in SPM and that perylene could be taken as an index to assess the contribution of river inflow to the total PAHs in SPM samples. The high concentration of perylene in the sediment was indicative of an in situ biogenic origin.  相似文献   

5.
The vertical concentration profiles and source contributions of polycyclic aromatic hydrocarbons (PAHs) and n-alkanes in respirable particle samples (PM4) collected at 10, 100, 200 and 300-m altitude from the Milad Tower of Tehran, Iran during fall and winter were investigated. The average concentrations of total PAHs and total n-alkanes were 16.7 and 591 ng/m3, respectively. The positive matrix factorization (PMF) model was applied to the chemical composition and wind data to apportion the contributing sources. The five PAH source factors identified were: ‘diesel’ (56.3 % of total PAHs on average), ‘gasoline’ (15.5 %), ‘wood combustion, and incineration’ (13 %), ‘industry’ (9.2 %), and ‘road soil particle’ (6.0 %). The four n-alkane source factors identified were: ‘petrogenic’ (65 % of total n-alkanes on average), ‘mixture of petrogenic and biomass burning’ (15 %), ‘mixture of biogenic and fossil fuel’ (11.5 %), and ‘biogenic’ (8.5 %). Source contributions by wind sector were also estimated based on the wind sector factor loadings from PMF analysis. Directional dependence of sources was investigated using the conditional probability function (CPF) and directional relative strength (DRS) methods. The calm wind period was found to contribute to 4.4 % of total PAHs and 5.0 % of total n-alkanes on average. Highest average concentrations of PAHs and n-alkanes were found in the 10 and 100 m samples, reflecting the importance of contributions from local sources. Higher average concentrations in the 300 m samples compared to those in the 200 m samples may indicate contributions from long-range transport. The vertical profiles of source factors indicate the gasoline and road soil particle-associated PAHs, and the mixture from biogenic and fossil fuel source-associated n-alkanes were mostly from local emissions. The smaller average contribution of diesel-associated PAHs in the lower altitude samples also indicates that the restriction of diesel-fueled vehicle use in the central area of Tehran has been effective in reducing the PAHs concentration.  相似文献   

6.
A method for compound-specific stable carbon isotope analysis of atmospheric polycyclic aromatic hydrocarbons (PAHs) in carbonaceous aerosols is described. Atmospheric aerosol samples containing PAHs (C-10 to C-20) were collected on filters using a high-volume sampling technique, solvent extracted, taken through a cleanup procedure, separated by gas chromatography, oxidized to CO2 on-line, and introduced into an isotope ratio mass spectrometer for analysis. The method can be used to determine the isotope composition of a few nanograms of PAHs. This technique was used to analyse and compare the isotope composition of atmospheric PAHs from standards, as well as two samples from urban and rural locations. Isotopic variability in atmospheric PAHs is greater than measurement uncertainties which makes this a potentially useful technique for source identification when used together with concentration measurements.  相似文献   

7.
Abstract

This study investigates the combustion kinetics and emission factors of 16 U.S. Environmental Protection Agency priority polycyclic aromatic hydrocarbons (PAHs) in polylactic acid (PLA) combustion. Experimentally, two reactions are involved in the PLA combustion process that potentially result in the release of lactide, acetaldehyde, and n-hexaldehyde. The products may continuously be oxidized to form carbon dioxide (CO2) and some PAHs produced because of incomplete combustion. The analytical results indicate that the emission factors for PAHs are in the range of not detectable to 98.04 μg/g. The emission factors are much lower than those of poly(ethylene terephalate) (PET) and other combustion of plastics. Results from this work suggest that combustion is a good choice for waste PLA disposal.  相似文献   

8.
Sharma H  Jain VK  Khan ZH 《Chemosphere》2007,66(2):302-310
This paper reports on polycyclic aromatic hydrocarbons (PAHs) in the atmospheric particulate matter of Jawaharlal Nehru University campus, an urbanized site of New Delhi, India. Suspended particulate matter samples of 24h duration were collected on glass-fiber filter paper for four representative days in each month during January 2002 to December 2003. PAHs were extracted from filter papers using toluene with ultrasonication method and analysed. Quantitative measurements of polycyclic aromatic hydrocarbons (PAHs) were carried out using the gas chromatography technique. The annual average concentration of total PAHs were found to be 668+/-399 and 672+/-388 ng/m3 in the years 2002 and 2003, respectively. The seasonal average concentrations were found to be maximum in winter and minimum during in the monsoon. The results of principal component analysis (PCA) indicate that diesel and gasoline driven vehicles are the principal sources of PAHs in all the seasons. In winter coal and wood combustion also significantly contribute to the PAH levels.  相似文献   

9.
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.  相似文献   

10.
Yang HH  Chen CM 《Chemosphere》2004,56(10):879-887
The application of a chemical mass balance air pollution model to ambient measurements of polycyclic aromatic hydrocarbons (PAHs) is presented. Sixteen air samples were collected at seven sites in a suburban area in Taiwan and analyzed for the concentration of 21 compounds between July 2001 and September 2001. Each ambient sample was evaluated for the PAH contribution from six sources (heavy oil combustion, natural gas combustion, coal combustion, diesel combustion, vehicles and municipal solid waste incinerator). Average predictions agree well with the emission inventory. By this method, the average contributions are 49%, 14%, 22%, 12%, and 2% from vehicles, heavy oil combustion, natural gas combustion, coal combustion and diesel combustion at these seven receptors. By far, vehicles are the major PAH emission sources and municipal solid waste incinerator is a minor contributor. The calculated result of particulate PAHs is compared with that of total (gaseous and particulate) PAHs. The estimate based on total PAHs is better than the estimate based on particulate PAHs only. Contributions of eight low reactive PAHs for the same emission sources and receptors were calculated. Atmospheric reactivity seems not a problem for source apportionment in this study.  相似文献   

11.
This study identifies major contributing sources of high particulate matter (PM) days in Hong Kong and conducive meteorological conditions leading to high PM. The PM10 chemical composition of 3393 ambient samples collected at ten monitoring stations in Hong Kong during 1998–2005 were used as input for positive matrix factorization (PMF) modeling to identify and quantify the aerosol sources in Hong Kong. Days with PM10 levels exceeding 56 μg m?3, the average plus one standard deviation of the mass concentration of all samples, are defined as high PM days. A total of 401 samples fell in the high PM category during the study period. Biomass burning, secondary sulfate and secondary nitrate were found to be the major contributors leading to high PM, responsible for 68–73% of PM10 mass on high PM days. The contributions by these sources on high PM days were 140–180% higher than their respective average concentration contributions. These sources were identified to be regional sources on the grounds of little spatial variation in their concentrations among the monitoring stations and a temporal pattern of higher in the winter and lower in the summer. Sampling days of high PM in 2004 and 2005 were individually examined for weather charts and regional surface wind maps. Weak high pressures over mainland China were the most important synoptic event leading to high PM days in the fall and winter, while typhoon episodes were responsible for most summer cases. Approximately 80% of the high PM days were in the fall and winter months (September–February). Almost all the high PM days were associated with northwesterly, northerly or northeasterly regional transport. Anthropogenic primary sources (coal combustion, vehicular exhaust, and residue oil combustion) showed the highest contributions associated with northwesterly wind, indicating the strong influence of the more urbanized areas to the northwest of Hong Kong in the Pearl River Delta region.  相似文献   

12.
Air samples were collected using active samplers at various heights of 8, 15, 32, 47, 65, 80, 102, 120, 140, 160, 180, 200, 240, 280 and 320 m on a meteorological tower in an urban area of Beijing in two campaigns in winter 2006. Altitudinal distributions of polycyclic aromatic hydrocarbons (PAHs) in atmospheric boundary layer of Beijing in winter season were investigated. Meteorological conditions during the studied period were characterized by online measurements of four meteorological parameters as well as trajectory calculation. The mean total concentrations of 15 PAHs except naphthalene of gaseous and particulate phase were 667±450 and 331±144 ng m−3 in January and 61±19 and 29±6 ng m−3 in March, respectively. Domestic coal combustion and vehicle emission were the dominant PAH sources in winter. Although the composition profiles derived from the two campaigns were similar, the concentrations were different by one order of magnitude. The higher concentrations in January were partly caused by higher emission due to colder weather than March. Moreover, weak wind, passing through the city center before the sampling site, picked up more contaminants on the way and provided unfavorable dispersion condition in January. For both campaigns, PAH concentrations decreased with heights because of ground-level emission and unfavorable dispersion conditions in winter. The concentration ratio of PAHs in gas versus solid phases was temperature dependent and negatively correlated to their octanol–air partition coefficients.  相似文献   

13.
From 28 November to 23 December 2009, 24-h?PM2.5 samples were collected simultaneously at six sites in Guangzhou. Concentrations of 18 polycyclic aromatic hydrocarbons (PAHs) together with certain molecular tracers for vehicular emissions (i.e., hopanes and elemental carbon), coal combustion (i.e., picene), and biomass burning (i.e., levoglucosan) were determined. Positive matrix factorization (PMF) receptor model combined with tracer data was applied to explore the source contributions to PAHs. Three sources were identified by both inspecting the dominant tracer(s) in each factor and comparing source profiles derived from PMF with determined profiles in Guangzhou or in the Pearl River Delta region. The three sources identified were vehicular emissions (VE), biomass burning (BB), and coal combustion (CC), accounting for 11?±?2 %, 31?±?4 %, and 58?±?4 % of the total PAHs, respectively. CC replaced VE to become the most important source of PAHs in Guangzhou, reflecting the effective control of VE in recent years. The three sources had different contributions to PAHs with different ring sizes, with higher BB contributions (75?±?3 %) to four-ring PAHs such as pyrene and higher CC contributions (57?±?4 %) to six-ring PAHs such as benzo[ghi]perylene. Temporal variations of VE and CC contributions were probably caused by the change of weather conditions, while temporal variations of BB contributions were additionally influenced by the fluctuation of BB emissions. Source contributions also showed some spatial variations, probably due to the source emission variations near the sampling sites.  相似文献   

14.
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.  相似文献   

15.
Three mercury (Hg) species (gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and fine particulate-bound mercury (PBM2.5)) were measured in the stack of a small scale wood combustion chamber at 400 °C, in the stack of an advanced wood boiler, and in two areas influenced by wood combustion. The low temperature process (lab-scale) emitted mostly GEM (∼99% when burning wood pellets and ∼95% when burning unprocessed wood). The high temperature wood boiler emitted a greater proportion of oxidized Hg (approximately 65%) than the low temperature system. In field measurements, mean PBM2.5 concentrations at the rural and urban sites in winter were statistically significantly higher than in warmer seasons and were well correlated with Delta-C concentrations, a wood combustion indictor measured by an aethalometer (UV-absorbable carbon minus black carbon). Overall the results suggest that wood combustion may be an important source of oxidized mercury (mostly in the particulate phase) in northern climates in winter.  相似文献   

16.
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.  相似文献   

17.
The aerosol samples were collected from a high elevation mountain site, Nainital, in India (1958 m asl) during September 2006 to June 2007 and were analyzed for water-soluble inorganic species, total carbon, nitrogen, and their isotopic composition (δ13C and δ15N, respectively). The chemical and isotopic composition of aerosols revealed significant anthropogenic influence over this remote free-troposphere site. The amount of total carbon and nitrogen and their isotopic composition suggest a considerable contribution of biomass burning to the aerosols during winter. On the other hand, fossil fuel combustion sources are found to be dominant during summer. The carbon aerosol in winter is characterized by greater isotope ratios (av. ?24.0?‰), mostly originated from biomass burning of C4 plants. On the contrary, the aerosols in summer showed smaller δ13C values (?26.0?‰), indicating that they are originated from vascular plants (mostly of C3 plants). The secondary ions (i.e., SO4 2?, NH4 +, and NO3 ?) were abundant due to the atmospheric reactions during long-range transport in both seasons. The water-soluble organic and inorganic compositions revealed that they are aged in winter but comparatively fresh in summer. This study validates that the pollutants generated from far distant sources could reach high altitudes over the Himalayan region under favorable meteorological conditions.  相似文献   

18.
Vapor- and particulate-phase polycyclic aromatic hydrocarbon (PAH) samples were continuously collected at an urban site in Dalian, China, during the heating and non-heating period. There is strong temperature dependence and obvious seasonal trend for atmospheric PAHs, and significant positive correlations of atmospheric PAHs with SO2 and CO concentrations were observed. Factor analysis model with non-negative constraints (FA–NNC) combined with local and literature PAH source fingerprints was successful in source identification of particulate PAHs in the atmospheric samples. The results suggested that, in heating period, the main pollution sources were identified as coal-fired boiler emission (56%), residential coal combustion (33%) and traffic emissions (11%). As for non-heating period, the main sources were gasoline engine emission, traffic tunnel emission and coal-fired power plant, and the overall source contributions of traffic emission (gasoline engine + traffic tunnel) were 79% and coal-fired power plant 21%. The current results support our previous study and provide new insights. This can be the first attempt to quantitatively apportion air organic pollutants using receptor models combined with local source fingerprints. The source fingerprints can be used as reference data for source apportionment of atmospheric PAHs of China.  相似文献   

19.
《Environmental Forensics》2013,14(3):191-197
To determine whether polycyclic aromatic hydrocarbons (PAHs) in household soot were derived from the combustion of scrap wood or creosote that was impregnated in the wood (or some combination of both), the molecular composition and radiocarbon ( 14 C) content of the total carbon and several PAHs in the soot was investigated. The 5730-year half-life of 14 C makes it an ideal marker for identifying creosote-derived PAHs ( 14 C-free) versus those derived from the combustion of wood (contemporary 14 C). The 14 C abundance of phenanthrene, fluoranthene, pyrene, and retene was determined by accelerator mass spectrometry after solvent extraction and purification by preparative capillary gas chromatography. The molecular analysis (presence of retene and 1,7-dimethylphenanthrene) and bulk 14 C content (contemporary) of the soot indicated that wood combustion was a strong source of carbon to the soot. The 14 C of retene in two soot samples was also contemporary, indicating that it was derived from the combustion of the scrap wood. These results are consistent with previous work that has suggested that retene is an excellent marker of wood combustion. However, the 14 C content of phenanthrene, fluoranthene, and pyrene in one soot sample was much lower and revealed that these compounds had a mixed creosote and wood source. Using an isotopic mass balance approach, we estimate that 40 to 70% of phenanthrene, fluoranthene, and pyrene were derived from the combustion of the scrap wood. The results of this study show that molecular marker and bulk 14 C analysis can be potentially misleading in apportioning sources of every PAH, and that molecular-level 14 C analysis of PAHs can be a powerful tool for environmental forensics.  相似文献   

20.
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 (PM0.4). In the latter category, not only were more PAHs present in PM0.4, but also contained higher fractions of high molecular weight PAHs. Generally, there were more than 89% of total particulate phase PAHs associated with PM2.5. 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.  相似文献   

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