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1.
Samples of ambient air (including gaseous and particulate phases), dust fall, surface soil, rhizosphere soil, core (edible part), outer leaf, and root of cabbage from eight vegetable plots near a large coking manufacturer were collected during the harvest period. Concentrations, compositions, and distributions of parent PAHs in different samples were determined. Our results indicated that most of the parent PAHs in air occurred in the gaseous phase, dominated by low molecular weight (LMW) species with two to three rings. Specific isomeric ratios and principal component analysis were employed to preliminarily identify the local sources of parent PAHs emitted. The main emission sources of parent PAHs could be apportioned as a mixture of coal combustion, coking production, and traffic tailing gas. PAH components with two to four rings were prevailing in dust fall, surface soil, and rhizosphere soil. Concentrations of PAHs in surface soil exhibited a significant positive correlation with topsoil TOC fractions. Compositional profiles in outer leaf and core of cabbage, dominated by LMW species, were similar to those in the local air. Overall, the order of parent PAH concentration in cabbage was outer leaf > root > core. Partial correlation analysis and multivariate linear stepwise regression revealed that PAH concentrations in cabbage core were closely associated with PAHs present both in root and in outer leaf, namely, affected by adsorption, then absorption, and translocation of PAHs from rhizosphere soil and ambient air, respectively.  相似文献   

2.
Passive samplers with polyurethane disks (PUF) were applied in the determination of the concentration of polycyclic aromatic hydrocarbons (PAHs) in ambient air in six residential areas in the Philippines during four simultaneous sampling periods. The uptake profiles of PAHs were determined at one site during one sampling period. Most of the PAHs that were detected in air at concentrations that were significantly higher than their analytical detection limits exhibited a linear uptake trend on the PUF disk. The linear uptake profiles of some high molecular weight (HMW) PAHs were not established and this is attributed to the low concentration of the compounds in air in the gaseous phase. The retention concentrations of phenanthrene-d-10 were determined after depuration in four sampling sites during two sampling periods. The sampling rate for phenanthrene-d-10 was calculated at the linear phase of the uptake using the kA derived from depuration experiments and the relationship of kA and sampling rate which was established in a previous passive sampling study. The average sampling rate obtained for phenanthrene d-10 (2.94±0.69 m3 d−1) was applied for derivation of the concentrations of the PAHs in the field samples.The passive sampler with PUF disk and short integration time of 42–56 days is applicable for the derivation of the concentrations of PAHs in ambient air in the Philippines. The concentrations of the organic pollutants derived from the passive sampler showed variability for the six residential areas; reflecting the influence of possible sources of emission of the pollutants at the sites at the different sampling periods. The weather conditions, including the occurrence of a tropical cyclone, increased rainfall and high-relative humidity during the rainy season, had an influence on the concentrations of PAHs derived by the passive sampler.  相似文献   

3.
Passive air sampling theory for semivolatile organic compounds   总被引:2,自引:0,他引:2  
The mathematical modelling underlying passive air sampling theory can be based on mass transfer coefficients or rate constants. Generally, these models have not been inter-related. Starting with basic models, the exchange of chemicals between the gaseous phase and the sampler is developed using mass transfer coefficients and rate constants. Importantly, the inter-relationships between the approaches are demonstrated by relating uptake rate constants and loss rate constants to mass transfer coefficients when either sampler-side or air-side resistance is dominating chemical exchange. The influence of sampler area and sampler volume on chemical exchange is discussed in general terms and as they relate to frequently used parameters such as sampling rates and time to equilibrium. Where air-side or sampler-side resistance dominates, an increase in the surface area of the sampler will increase sampling rates. Sampling rates are not related to the sampler/air partition coefficient (K(SV)) when air-side resistance dominates and increase with K(SV) when sampler-side resistance dominates.  相似文献   

4.
A passive air sampler was developed for collecting polycyclic aromatic hydrocarbons (PAHs) in air mass from various directions. The airflow velocity within the sampler was assessed for its responses to ambient wind speed and direction. The sampler was examined for trapped particles, evaluated quantitatively for influence of airflow velocity and temperature on PAH uptake, examined for PAH uptake kinetics, calibrated against active sampling, and finally tested in the field. The airflow volume passing the sampler was linearly proportional to ambient wind speed and sensitive to wind direction. The uptake rate for an individual PAH was a function of airflow velocity, temperature and the octanol-air partitioning coefficient of the PAH. For all PAHs with more than two rings, the passive sampler operated in a linear uptake phase for three weeks. Different PAH concentrations were obtained in air masses from different directions in the field test.  相似文献   

5.
Concentrations of polycyclic aromatic hydrocarbons (PAHs) were measured in soil and XAD-based passive air samples taken from a total of 22 sites along three transects (Revelstoke, Yoho, and Observation, 6-8 sites for each transect) in the mountains of Western Canada in 2003-2004. Median concentrations in air (4-ring PAHs: 33 pg/m3) were very low and comparable to those in global background regions such as the Arctic. Low median soil concentrations (16 EPA PAHs: 16 ng/g dry weight) and compositional profiles dominated by naphthalene and phenanthrene are similar to those of tropical soils, indicative of remote regions influenced mostly by PAHs from traffic and small settlements. Comparing levels and composition of PAHs in soils between and along transects indeed suggests a clear relationship with proximity to local sources. Sampling sites that are closer to major traffic arteries and local settlements have higher soil concentrations and a higher relative abundance of heavier PAHs than truly remote sites at higher elevations. This remains the case when the variability in soil organic carbon content between sites is taken into account. Both air/soil concentration ratios and fugacity fractions suggest atmospheric net deposition of four-ring PAHs to soils.  相似文献   

6.
Uptake of vapor and particulate polycyclic aromatic hydrocarbons by cabbage   总被引:1,自引:0,他引:1  
Polycyclic aromatic hydrocarbons (PAHs) in cabbage (aerial part), air (gas and particles) and soil samples collected from two sites in Tianjin, China were measured. Although the levels of PAHs in all samples from the heavily contaminated site B were higher than those from the less contaminated site A, the PAH profiles were similar, suggesting the similarity in source type. PAH concentrations in cabbages were positively correlated to either gas or particle-bound PAHs in air. A multivariate linear regression with cabbage PAH as a function of both gas and particle-bound PAHs in air was established to quantitatively characterize the relationship between them. Inclusion of soil PAH concentrations would not improve the model, indicating that the contribution of soil PAHs to cabbage (aerial part) accumulation was insignificant.  相似文献   

7.
This study aimed to characterize air pollution and the associated carcinogenic risks of polycyclic aromatic hydrocarbon (PAHs) at an urban site, to identify possible emission sources of PAHs using several statistical methodologies, and to analyze the influence of other air pollutants and meteorological variables on PAH concentrations.The air quality and meteorological data were collected in Oporto, the second largest city of Portugal. Eighteen PAHs (the 16 PAHs considered by United States Environment Protection Agency (USEPA) as priority pollutants, dibenzo[a,l]pyrene, and benzo[j]fluoranthene) were collected daily for 24 h in air (gas phase and in particles) during 40 consecutive days in November and December 2008 by constant low-flow samplers and using polytetrafluoroethylene (PTFE) membrane filters for particulate (PM10 and PM2.5 bound) PAHs and pre-cleaned polyurethane foam plugs for gaseous compounds. The other monitored air pollutants were SO2, PM10, NO2, CO, and O3; the meteorological variables were temperature, relative humidity, wind speed, total precipitation, and solar radiation. Benzo[a]pyrene reached a mean concentration of 2.02 ng?m?3, surpassing the EU annual limit value. The target carcinogenic risks were equal than the health-based guideline level set by USEPA (10?6) at the studied site, with the cancer risks of eight PAHs reaching senior levels of 9.98?×?10?7 in PM10 and 1.06?×?10?6 in air. The applied statistical methods, correlation matrix, cluster analysis, and principal component analysis, were in agreement in the grouping of the PAHs. The groups were formed according to their chemical structure (number of rings), phase distribution, and emission sources. PAH diagnostic ratios were also calculated to evaluate the main emission sources. Diesel vehicular emissions were the major source of PAHs at the studied site. Besides that source, emissions from residential heating and oil refinery were identified to contribute to PAH levels at the respective area. Additionally, principal component regression indicated that SO2, NO2, PM10, CO, and solar radiation had positive correlation with PAHs concentrations, while O3, temperature, relative humidity, and wind speed were negatively correlated.  相似文献   

8.
Semipermeable membrane devices (SPMDs) were used for measurements in air of twelve polycyclic aromatic hydrocarbons (PAHs) in two Genoa locations, both on building roofs, distant 300 m from each other. The first, site A, was in front a dismissing steel complex and the second, site B, was in an urban area overlooking a busy thoroughfare. SPMDs were deployed contemporary at the two sites, in nine monthly samplings, from April 2007 to May 2008. The amount of sequestered PAHs, in sites A and B, ranged between 61–267 ng SPMD?1 d?1 and 50–535 ng SPMD?1 d?1, respectively.PAHs profiles highlighted seasonal differences and suggested the possible role of different PAHs sources in the two areas. In particular, the contribution of remediation works of the steel complex was observed in site A. Moreover, a naphthalene leak from a tank, into the former industrial area, and a fire broke out near site A, were registered by time-integrated measurements of SPMDs.However, the strong dependence between amount of sequestered PAHs and air temperature needs further studies to distinguish between uptake rate variability and seasonal contribution of different sources. Finally, to measure air concentrations with reasonable accuracy, it should be very important to have certified sampling rates for all individual PAHs.  相似文献   

9.
We examined PAH uptake by Norway spruce needles following the emergence of new buds in spring 2004–June 2005. Atmospheric PAH concentrations (gaseous phase and particle-bound) were monitored during this period, and PAH concentrations from these three environmental media were then used to calculate deposition and transfer velocities. Benzo(a)pyrene was found almost exclusively associated to particles and thus was used to determine a particle-bound deposition velocity of 10.8 m h?1. PAHs present in both compartments had net gaseous transfer velocities ranging from negligible values to 75.6 m h?1 and correlated significantly with log KOA. The loss velocities thereafter calculated were found to be higher for more volatile PAHs. Using the calculated average atmospheric PAH concentrations and deposition velocities, it was thus possible to model PAH uptake by vegetation through time. We demonstrate that this approach can be used to determine deposition velocities without the use of a surrogate surface. In considering both particulate-bound and gaseous deposition processes this model can be used not only to study air–foliage exchange of semi-volatile organic compounds, but also to illustrate the relative contribution of gaseous deposition and particulate-bound deposition in the overall atmospheric vegetation uptake of semi-volatile organic compounds.  相似文献   

10.
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.  相似文献   

11.
A 14-week filter pack (FP) sampler evaluation field study was conducted at a site near Bondville, IL to investigate the impact of weekly sampling duration. Simultaneous samples were collected using collocated filter packs (FP) from two independent air quality monitoring networks (CASTNet and Acid-MODES) and using duplicate annular denuder systems (ADS). Precision estimates for most of the measured species are similar for weekly ADS and composited FPs. There is generally good agreement between the weekly CASTNet FP results aggregated from weekly daytime and weekly nighttime samples and those aggregated from daily 24 h Acid-MODES samples; although SO2 is the exception, and CASTNet concentrations are higher than Acid-MODES. Comparison of weekly ADS results with composited weekly FP results from CASTNet shows good agreement for SO2-4. With the exception of the two weeks where the FP exceeded the ADS, both HNO3 and the sum of particulate and gaseous NO-3 show good agreement. The FP often provides good estimates of HNO3, but when used to sample atmospheres that have experienced substantial photochemical reactivity, FP HNO3 determinations using nylon filters may be biased high. It is suggested that HNO2 or some other oxidized nitrogen compound can accumulate on a regional scale and may interfere with the FP determination of HNO3. FP particulate NO-3 results are in fair agreement with the ADS. Since FP SO2 results are biased low by 12–20%, SO2 concentration in the CASTNet data archive should be adjusted upward. Nylon presents problems as a sampling medium in terms of SO2 recovery and specificity for HNO3. Additional comparative sampler evaluation studies are recommended at several sites over each season to permit comprehensive assessment of the concentrations of atmospheric trace constituents archived by CASTNet.  相似文献   

12.
To investigate the characteristics of mercury exchange between soil and air in the heavily air-polluted area, total gaseous mercury (TGM) concentration in air and Hg exchange flux were measured in Wanshan Hg mining area (WMMA) in November, 2002 and July–August, 2004. The results showed that the average TGM concentrations in the ambient air (17.8–1101.8 ng m−3), average Hg emission flux (162–27827 ng m−2 h−1) and average Hg dry deposition flux (0–9434 ng m−2 h−1) in WMMA were 1–4 orders of magnitude higher than those in the background area. It is said that mercury-enriched soil is a significant Hg source of the atmosphere in WMMA. It was also found that widely distributed roasted cinnabar banks are net Hg sources of the atmosphere in WMMA. Relationships between mercury exchange flux and environmental parameters were investigated. The results indicated that the rate of mercury emission from soil could be accelerated by high total soil mercury concentration and solar irradiation. Whereas, highly elevated TGM concentrations in the ambient air can restrain Hg emission from soil and even lead to strongly atmospheric Hg deposition to soil surface. A great amount of gaseous mercury in the heavily polluted atmosphere may cycle between soil and air quickly and locally. Vegetation can inhibit mercury emission from soil and are important sinks of atmospheric mercury in heavily air-polluted area.  相似文献   

13.
A sampling system and analytical procedure for determining PCDD/Fs, PCBs, HCB, and PAHs in ambient air was tested. The reproducibility of the concentrations and the gas/particle partitioning was ± 10% for most compounds. The removal of gaseous compounds on the XAD resin trap was greater than 99%. The adsorption of gaseous substances on the glass fiber filter was negligible for compounds primarily found in the gas phase, but could not be ruled out for compounds found mainly on particles.  相似文献   

14.
A novel design of rapidly equilibrating passive air sampler was deployed at 38 sites across 19 European countries to investigate short-term spatial variability of persistent organic pollutants (POPs). Devices were sealed in airtight containers to eliminate the possibility of contamination during transit and couriered to recipients with deployment instructions. Exposure times of 7days permitted the use of back trajectory analysis to further understand the factors responsible for influencing the large-scale spatial distribution of PCBs, PBDEs, PCNs, PAHs, lindane and HCB. Following sampler harvest, devices were sealed and returned for analysis. Comparison of sequestered levels showed that PAHs exhibited the greatest spatial variability (by a factor of 30) with higher levels often associated with greater population density. In contrast, HCB values were much more uniform, reflecting its well mixed distribution in the atmosphere. Spatial variation was strongly influenced by air mass origin, with lower levels being observed at most sites impacted by maritime air masses.  相似文献   

15.
Surface soil and passive air samples from a network of 23 sampling sites across Costa Rica were analyzed for polycyclic aromatic hydrocarbons (PAHs), allowing for an evaluation of absolute levels, spatial distribution patterns, air/soil concentration (A/S) ratios and relative composition. Annual mean concentrations of four-ring PAHs in air were low (median of approximately 40 pg m−3), except in Costa Rica's densely populated central valley (approximately 650 pg m−3). PAH concentrations in soil were also low (median of 5 ng g−1 dry weight) and comparable to those reported for other tropical regions. These low soil concentrations result in A/S ratios of four-ring PAHs in Costa Rica that are higher than the equilibrium air–soil partitioning coefficients and also higher than A/S ratios reported for temperate locations. A series of model calculations of increasing complexity were used to seek an explanation for variable A/S ratios of PAHs under tropical and temperate conditions. Temperature-driven changes in air–soil partitioning and differences in PAH degradability under temperate and tropical conditions are insufficient to explain the higher soil concentrations and lower A/S ratios in temperate regions. However, these can be explained by atmospheric deposition of PAHs during historical periods of much higher emissions and air concentrations and by persistence of PAHs in soils on the order of decades. Low PAH concentrations in tropical soils were found to be consistent with constant or increasing emissions, and in particular, do not require that degradation rates in soil are much faster than in temperate areas. In comparison to temperate soils, soils from Costa Rica and other tropical regions have a higher relative abundance of the lighter PAHs. This likely reflects a higher source contribution from biomass burning in the tropics, as well as the preferential loss of lighter PAHs from temperate soils that experienced high PAH deposition in the past.  相似文献   

16.
From 1994 to 2003, daily air concentrations of particle-bound polycyclic aromatic hydrocarbons (PAHs) and carbon monoxide (CO) were regularly monitored at two traffic-oriented sampling sites (A and B) in urban Genoa, Italy. The data were used to estimate effects on air quality in real situations due to progressive substitution of EURO-0 vehicles, started in 1993, with less-polluting vehicles (EURO-1, EURO-2), mainly gasoline vehicles with a catalyst. PAH profile classification and diagnostic PAH ratios were used to identify 345 samples of predominantly traffic origin. At both sites, CO and PAH daily concentrations decreased exponentially with time and the apparent half-life values calculated were 6.3 and 5.5 for CO and 3.7 and 3.5 years for PAHs at sites A and B, respectively. At site A, monitored for traffic intensity, multiple regression analyses confirmed that daily PAH and CO concentrations were positively correlated with the number of non-catalytic vehicles estimated to cross this site during sampling and negatively correlated with seasonal variables (air temperature, ozone concentration, relative air humidity). The reduction in air pollution estimated for complete substitution of non-catalytic gasoline vehicles was 89% for BaP, 85% for total PAHs and 69% for CO.  相似文献   

17.
The concentrations of 15 priority PAHs were determined in the atmospheric gaseous and particulate phases from nine sites across Assiut City, Egypt. While naphthalene, acenaphthene, and fluorene were the most abundant in the gaseous phase with average concentrations of 377, 184, and 181 ng/m3, benzo[b]fluoranthene, chrysene, and benzo[g,h,i]perylene showed the highest levels in the particulate phase with average concentrations of 76, 6, and 52 ng/m3. The average total atmospheric concentration of target PAHs (1,590 ng/m3) indicates that Assiut is one of the highest PAH-contaminated areas in the world. Statistical analysis revealed a significant difference between the levels of PAHs in the atmosphere of urban and suburban sites (P?=?0.029 and 0.043 for gaseous and particulate phases, respectively). Investigation of diagnostic PAH concentration ratios revealed vehicular combustion and traffic exhaust emissions as the major sources of PAHs with a higher contribution of gasoline rather than diesel vehicles in the sampled areas. Benzo[a]pyrene has the highest contribution (average?=?32, 4 % for gaseous and particulate phases) to the total carcinogenic activity (TCA) of atmospheric PAHs. While particulate phase PAHs have higher contribution to the TCA, gaseous phase PAHs present at higher concentrations in the atmosphere are more capable of undergoing atmospheric reactions to form more toxic derivatives.  相似文献   

18.
Surface and core sediments collected from six fish farms in Hong Kong and from reference sites were investigated for the enrichment and sources of polycyclic aromatic hydrocarbons (PAHs). Moderately high ∑PAH16 levels (123-947 ng g−1, mean: 450 ng g−1) were found in the surface aquaculture sediments. In comparison with the sediments from the reference sites, the average enrichment percentage of total organic carbon (TOC) and PAHs in surface sediments were 21.4 and 43.8%, respectively, and in the core sediments, 24.6 and 73.7%, respectively. Mathematical source apportionment analyses (i.e. isomer ratios, hierarchical cluster analysis, principal components analysis with multiple linear regression analysis) suggested a higher percentage of petrogenic sources in aquaculture sediments. The fish feeds might be the main source of the enriched PAHs in the aquaculture sediments. To our knowledge, this is the first study showing that PAHs in aquaculture sediments could be attributed to human aquaculture activities.  相似文献   

19.
Ambient air samples from a traffic intersection, an urban site and a petrochemical-industrial site (PCI) were collected by using several dry deposition plates, two Microorifice uniform deposited impactors (MOUDIs), one Noll Rotary Impactor (NRI) and several PS-1 (General Metal Work) samplers from March 1994 to June 1995 in southern Taiwan, to characterize the atmospheric particle-bound PAH content of these three areas. Twenty-one individual polycyclic aromatic hydrocarbons (PAHs) were analyzed primarily by using a gas chromatograph/mass spectrometer (GC/MS). In general, the sub-micron particles have a higher PAH content. This is due to the fact that soot from combustion sources consists primarily of fine particles and has a high PAH content. In addition, a smaller particle has a higher specific surface area and therefore may contain more organic carbon, which allows for more PAH adsorption. For a particle size range between 0.31 and 3.2 microm, both Urban/Traffic and PCI/Traffic ratios of particle-bound total-PAH content have the lowest values, ranging from 0.25 to 0.28 (mean = 0.26) and from 0.07 to 0.13 (mean = 0.10), respectively. This indicates that, during the accumulation process, the PAH mass shifted from a particle phase to a gas phase, or the particles aggregated with lower PAH-content particles, resulting in a reduction in particle-bound PAH content. By using the particle size distribution data, the dry deposition model in this study can provide a good prediction for the PAH content of dry deposition materials. In general, lower molecular weight PAHs had a larger fraction of dry deposition flux contributed by the gas phase; for 2-ring PAH (50.4, 46.3 and 28.4%), 3-ring PAHs (15.2, 15.4 and 11.7%) and 4-ring PAHs (13.0, 3.60 and 5.01%) for the traffic intersection, urban and PCI sites, respectively. For higher molecular weight PAHs-5-ring, 6-ring and 7-ring PAHs-their cumulation fraction (F%) of dry deposition flux contributed by the gas phase was lower than 3.26%. At the traffic intersection, urban and PCI sites, the mass median diameter of dry deposition materials (MMD(F)) of individual PAHs was between 25.3 and 49.6 microm, between 27.6 and 43.9 microm, and between 19.1 and 41.9 microm, respectively. This is due to the fact that PAH dry-deposition primarily resulted from gravitational settling of the coarse particulates (> 10 microm).  相似文献   

20.
For over one year, the Environmental Protection Commission of Hillsborough County (EPCHC) in Tampa, Florida, operated two dichotomous sequential particulate matter air samplers collocated with a manual Federal Reference Method (FRM) air sampler at a waterfront site on Tampa Bay. The FRM was alternately configured as a PM2.5, then as a PM10 sampler. For the dichotomous sampler measurements, daily 24-h integrated PM2.5 and PM10–2.5 ambient air samples were collected at a total flow rate of 16.7 l min−1. A virtual impactor split the air into flow rates of 1.67 and 15.0 l min−1 onto PM10–2.5 and PM2.5 47-mm diameter PTFE® filters, respectively. Between the two dichotomous air samplers, the average concentration, relative bias and relative precision were 13.3 μg m−3, 0.02% and 5.2% for PM2.5 concentrations (n=282), and 12.3 μg m−3, 3.9% and 7.7% for PM10–2.5 concentrations (n=282). FRM measurements were alternate day 24-h integrated PM2.5 or PM10 ambient air samples collected onto 47-mm diameter PTFE® filters at a flow rate of 16.7 l min−1. Between a dichotomous and a PM2.5 FRM air sampler, the average concentration, relative bias and relative precision were 12.4 μg m−3, −5.6% and 8.2% (n=43); and between a dichotomous and a PM10 FRM air sampler, the average concentration, relative bias and relative precision were 25.7 μg m−3, −4.0% and 5.8% (n=102). The PM2.5 concentration measurement standard errors were 0.95, 0.79 and 1.02 μg m−3; for PM10 the standard errors were 1.06, 1.59, and 1.70 μg m−3 for two dichotomous and one FRM samplers, respectively, which indicate the dichotomous samplers have superior technical merit. These results reveal the potential for the dichotomous sequential air sampler to replace the combination of the PM2.5 and PM10 FRM air samplers, offering the capability of making simultaneous, self-consistent determinations of these particulate matter fractions in a routine ambient monitoring mode.  相似文献   

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