Sulfate Emissions from Catalyst-Equipped Automobiles on the Highway

Abstract

A systematic investigation of solid and gaseous atmospheric emissions from some coke-oven batteries of one of Europe’s largest integrated steel factory (Taranto, Italy) has been carried out. In air monitoring samples, polycyclic aromatic hydrocarbons (PAHs) were consistently detected at concentrations largely exceeding threshold limit values. By means of PAHs speciation profile and benzo (a)pyrene (BaP) equivalent dispersion modeling from diffuse sources, the study indicated that serious health risks exist not only in working areas, but also in a densely populated residential district near the factory.     

Polycyclic aromatic hydrocarbons (PAHs) and their oxygen-containing derivatives (OPAHs) in soils from the Angren industrial area, Uzbekistan

We measured the concentrations and depth distribution (0-10, 10-20 cm) of 31 PAHs and 12 OPAHs in soils at eleven equidistant sampling points along a 20-km transect in the Angren industrial region (coal mine, power plant, rubber factory, gold mine), Uzbekistan to gain an insight into their concentrations, sources, and fate. Concentrations of all compounds were mostly much higher in the 0-10 cm than in the 10-20 cm layer except in disturbed soil close to the coal mine. Proximity to one of the industrial emitters was the main determinant of PAH and OPAH concentrations. The ∑31PAHs concentrations correlated positively with the ∑7 carbonyl-OPAH (r = 0.98, p < 0.01), ∑5 hydroxyl-OPAH (r = 0.72, p < 0.05), and with industrially emitted trace metals in the topsoil, identifying industrial emissions as their common source. Concentrations of several OPAHs were higher than their parent PAHs, but their vertical distribution in soil suggested only little higher mobility of OPAHs than their corresponding parent PAHs.     

The use of mosses and pine needles to detect persistent organic pollutants at local and regional scales

Polycyclic aromatic hydrocarbons (PAHs) were analysed in mosses (Hypnum cupressiforme) and pine needles (Pinus sylvestris) collected in the Czech Republic between 1988-94 at a regional background site in Kosetice, south Bohemia (1988-94) and two industrial sources. One industrial site (sampled 1989-91) in middle Moravia, was near a factory producing PAHs, carbon black and phthalates, the other (sampled 1991-93) near a coal and gas fuel production plant in western Bohemia. Selected chlorinated pesticides and polychlorinated biphenyl congeners were also analysed in samples at the regional background site. This study clearly shows that vegetation sampling can be used to show spatial differences in the atmospheric burden of a range of persistent organic pollutants with differences in the mixtures of compounds reflecting differences in their regional or local use/atmospheric emission.     

Estimation of PAHs dry deposition and BaP toxic equivalency factors (TEFs) study at Urban, Industry Park and rural sampling sites in central Taiwan, Taichung

The concentrations of polycyclic aromatic hydrocarbons (PAHs) in gas phase and particle bound were measured simultaneously at industrial (INDUSTRY), urban (URBAN), and rural areas (RURAL) in Taichung, Taiwan. And the PAH concentrations, size distributions, estimated PAHs dry deposition fluxes and health risk study of PAHs in the ambient air of central Taiwan were discussed in this study. Total PAH concentrations at INDUSTRY, URBAN, and RURAL sampling sites were found to be 1650 +/- 1240, 1220 +/- 520, and 831 +/- 427 ng/m3, respectively. The results indicated that PAH concentrations were higher at INDUSTRY and URBAN sampling sites than the RURAL sampling sites because of the more industrial processes, traffic exhausts and human activities. The estimation dry deposition and size distribution of PAHs were also studied. The results indicated that the estimated dry deposition fluxes of total PAHs were 58.5, 48.8, and 38.6 microg/m2/day at INDUSTRY, URBAN, and RURAL, respectively. The BaP equivalency results indicated that the health risk of gas phase PAHs were higher than the particle phase at three sampling sites of central Taiwan. However, compared with the BaP equivalency results to other studies conducted in factory, this study indicated the health risk of PAHs was acceptable in the ambient air of central Taiwan.     

Polycyclic aromatic hydrocarbons in the surface soils from outskirts of Beijing, China

Surface soils from the outskirts of Beijing were analyzed for 16 priority polycyclic aromatic hydrocarbons (PAHs) using gas chromatography and mass spectrometry (GC-MS). The distribution map of total PAHs content was obtained as a contour plot. The concentration range of 16 PAHs varied by over two orders of magnitude from 0.016 microg g-1 in rural to 3.884 microg g-1 in suburban soils with the relatively standard deviation of 70.5%, showing large differences in the extent of PAHs pollution at the various sampling sites. It was notable that the concentration of BaP was 0.005-0.270 microg g-1 with a mean of 0.055 microg g-1. In general, the distribution of PAHs centered on the high molecular weight PAHs known to be carcinogenic. The 4-6 ring PAHs represented about 66% in rural samples and 70% in suburban soils of the total PAHs found. There was relatively good relationship among most of the individual PAHs and the compounds of Pyr, BaA, Flu, BbF, BaP, Chr and Ph gave strong correlation (r>0.8) with the sum of PAHs. The selected marked compounds, a principal component analysis (PCA) and special PAHs compound ratios (Ph/An vs Flu/Pyr; summation operator COMB/ summation operator EPA-PAHs) suggest the pyrogenic origins, especially traffic exhausts, are the dominant sources of PAHs in Beijing outskirts soils.     

Risk based characterisation of contaminated industrial site using multivariate and geostatistical tools

Human and ecological risk assessment requires the sources, distribution, mobility and environmental behaviour of contaminants to be investigated on a site-specific basis. It often deals with data sets which are relatively small and affected by sampling gaps. In the case of a polycyclic aromatic hydrocarbon (PAH) contaminated industrial site, Kriging interpolation of spatial data and principal component analysis (PCA) proved useful for extracting additional value from the data set. Kriging was adopted for assessing the horizontal and vertical distribution and transport of PAHs in soil. PCA was applied to PAH concentration and relative abundance in soil samples and interpreted on the basis of the PAH physico-chemical and bio-degradation properties. It revealed correlation with the products of a neighbouring factory and the weathering of the lighter PAHs. The geo- and multivariate statistical results were coupled with the previous hydrogeological characterisation of the site to develop a site-conceptual model for use in the exposure scenario modelling for risk assessment.     

Distribution of polycyclic aromatic hydrocarbons in water, suspended particulate matter and sediment from Daliao River watershed, China

This study investigated the spatial distribution of polycyclic aromatic hydrocarbons (PAHs) in surface water, suspended particulate matter (SPM) and sediment of Daliao River watershed composed of the Hun River, Taizi River, and Daliao River. The sources of PAHs were evaluated employing ratios of specific PAHs compounds and principal component analysis (PCA). The total concentrations of PAHs ranged from 946.1 to 13448.5 ng l(-1) in surface water, from 317.5 to 238518.7 ng g(-1) dry weight in SPM, and from 61.9 to 840.5 ng g(-1) dry weight in sediments. The levels of PAHs are relatively higher in water and SPM, and lower in sediments, in comparison with those reported for other rivers and marine systems around the world. The composition of PAHs in these mediums was mainly 4-6 rings PAHs. The higher contents of low molecular weight PAHs in the water and SPM suggest a relatively recent local source of PAHs, entered into the river via wastewater discharge and atmospheric way. On the other hand, the heavy pollution of PAHs in sediment and water near heavy industrial area suggests that PAHs have been released from industrial wastewater.     

Long-range transport of polycyclic aromatic hydrocarbons from China to Japan

Airborne particulate matter was collected at Wajima, on the Noto Peninsula, Ishikawa, Japan by a high-volume air sampler with a quartz filter every week from 17 September 2004 to 16 September 2005. Polycyclic aromatic hydrocarbons (PAHs) extracted from filters were analyzed by HPLC with fluorescence detection. The atmospheric concentrations of PAHs at Wajima were higher during the heating period of China (when coal is burned for heat) than during the no-heating period. A meteorological analysis indicated that the air samples collected in that heating period at Wajima were transported mainly from Northeast China over the Japan Sea. Principal component analysis of nine PAHs indicated a Chinese origin of the PAHs. These results strongly suggest that the high-level PAHs detected at Wajima were the result of long-range transport from China.     

Assessment of the bioaccessibility of polycyclic aromatic hydrocarbons in soils from Beijing using an in vitro test

As an important human exposure pathway of contaminants, soil ingestion is of increasing concern for assessing health risk from polycyclic aromatic hydrocarbons (PAHs) in soils. A wide range of total PAH concentrations ranging from 0.112 microg g(-1) to 27.8 microg g(-1) in soils collected from different public sites, including gas stations, roadsides, bus stops, a kindergarten, primary and middle schools, a university and residential area, was detected. In general, total PAHs concentrations in soils from traffic areas were significantly higher than that from the other sites, indicating a dominant contribution from motor vehicles. Physiologically based in vitro tests were used to evaluate the oral bioaccessibility of PAHs in surface soil under different land uses in Beijing regarding both gastric and small intestinal conditions. It was found that the oral bioaccessibility of total PAHs in small intestinal condition, ranging from 9.2% to 60.5% of total PAHs in soil, was significantly higher than gastric condition, ranging from 3.9% to 54.9%. The bioaccessibility of individual PAHs in soils generally decreased with the increasing ring number of PAHs in both gastric and small intestinal conditions. However, the ratio of bioaccessibility of individual PAHs in gastric condition to that in small intestinal condition, generally increased with increasing ring number, indicating the relatively pronounced effect of bile extract on improving bioaccessibility of PAHs with relatively high ring numbers characterized by their high K(ow) values. The observation that bile extract at a level higher than critical micelle concentration could reduce the surface tension of digestive juice substantially, which may cause PAHs to be available for intestinal absorption, calls for more careful establishment of reliable soil criteria for PAHs, especially concerning the health of children who may ingest a considerable amount of PAH-contaminated soil via outdoor hand-mouth activities.     

Chemical characterization and source identification of polycyclic aromatic hydrocarbons in aerosols originating from different sources

To obtain the characteristic factors or signatures of particulate polycyclic aromatic hydrocarbons (PAHs) to help identify the sources of particulate PAHs in the atmosphere, different carbonaceous aerosols were generated by burning different fossil fuels and biomass under different conditions in the laboratory, and the chemical characteristics of 14 PAHs were studied in detail. The results showed that (1) carbonaceous aerosols derived from domestic burning of coal, diesel fuel, and gasoline have much higher concentrations of PAHs than those derived from domestic burning of biomass; (2) carbonaceous aerosols derived from domestic burning of diesel fuel/gasoline have similar PAH components as those derived from high-temperature combustion of diesel fuel/gasoline, although the former have much higher concentrations of PAHs than the latter, suggesting that the burning temperature obviously affects the emitting amount of particulate PAHs, but only slightly influences the PAHs components; and (3) the ratios of benzo[b]fluoranthene/acenaphthylene, benzo[b]fluoranthene/fluorene, dibenzo[a,h]anthracene/acenaphthylene, dibenzo[a,h]anthracene/fluorine, and benzo[b]fluoranthene/benzo[k]fluoranthene in carbonaceous aerosols are sensitively dependent on their sources, indicating that these ratios are suitable for use as characteristic factors or signatures of particulate PAHs in the atmosphere.     

Dissolution and removal of PAHs from a contaminated soil using sunflower oil

This study reports on the feasibility of remediation of polycyclic aromatic hydrocarbon (PAH) contaminated soils using sunflower oil, an environmentally-friendly solvent. Batch experiments were performed to test the influence of oil/soil ratio on the remediation of PAH contaminated soil, and to test the mass transfer behaviors of PAHs from soil to oil. An empirical model was employed to describe the kinetics of PAH dissolution and to predict equilibrium concentrations of PAHs in oil. PAH containing oil was regenerated using active carbon. Results show that dissolution of PAHs from a Manufactured Gas Plant (MGP) soil at oil/soil ratios of one or two were almost the same. Nearly all PAHs (81-100%) could be removed by sunflower oil dissolution. Mass transfer coefficients for low molecular PAHs namely fluoranthene, phenanthrene and anthracene were one or two orders of magnitude higher than those for high molecular PAHs with 4-6 rings. Ninety milliliters of PAH containing oil could be regenerated by 10 g active carbon in a batch reactor. Such a remediation procedure indicates that sunflower oil is a promising agent for the removal of PAHs from MGP soils. However, further research is required before the method can be used for in situ remediation of contaminated sites.     

Release of polycyclic aromatic hydrocarbons from Yangtze River sediment cores during periods of simulated resuspension

The role of resuspension duration on release of 16 PAHs was measured experimentally using a particle entrainment simulator (PES). Three sediment cores were resuspended for 12h at 0.2 and 0.5N m(-2). PAHs in water column and total suspended solids (TSS) were monitored at intervals. After 0.25h of resuspension, PAH release was on average 42% of their concentrations after 12h of resuspension, indicating fast release of PAHs from sediments in an initial short time. Moreover, PAHs released faster at 0.5N m(-2) than at 0.2N m(-2); low molecular weight PAHs (2-3-ring) released faster than median molecular weight (4-ring) PAHs. PAH concentrations in TSS showed generally increase with time and differences in magnitudes based on sediment type and energy. Overall, the composition of sediments is the major factor in determining the amount of released PAHs, more so than the level of resuspension energy applied.     

Occurrence and assessment of polycyclic aromatic hydrocarbons in soils from vegetable fields of the Pearl River Delta, South China

Surface soil (0-20 cm) samples from nine representative vegetable fields located in Guangzhou, Shenzhen, Zengcheng and Huadu within the Pearl River Delta, South China were collected and analyzed for 16 USEPA priority polycyclic aromatic hydrocarbons (PAHs) using gas chromatography coupled to mass spectrometry (GC-MS). Total concentrations of 16 PAHs (Sigma(PAHs)) ranged from 160 to 3700 microg kg(-1). Large variations were observed also between concentrations of individual PAHs from different vegetable fields and within the site as well. Acenapthylene, benzo[b]fluoranthene, fluoranthene, benzo[a]pyrene and benzo[k]fluoranthene were consistently the most prevalent individual PAHs. The values of PAH isomer ratios [anthracene/(anthracene+phenanthrene) and fluoranthene/(fluoranthene+pyrene)] indicate that combustion processes are the major sources of PAHs. Concentrations of PAHs were poorly correlated with organic carbon concentrations of soils, suggesting different sources and also indicating that the PAH pollution of this area is recent. The same outcome is confirmed by the predominance of PAHs with fewer rings (相似文献   

PAH removal from spiked municipal wastewater sewage sludge using biological, chemical and electrochemical treatments

Polycyclic aromatic hydrocarbons (PAHs) have been widely studied due to their presence in all the environmental media and toxicity to life. These molecules are strongly adsorbed on the particulate matters of soils, sludges or sediments because of their strong hydrophobicity which makes them less bioavailability, thus limiting their bioremediation. Different sludge treatment processes were tested to evaluate their performances for PAH removal from sludge prealably doped with 11 PAHs (5.5mg each PAH kg(-1) of dry matter (DM)): two biological processes (mesophilic aerobic digestion (MAD) and simultaneous sewage sludge digestion and metal leaching (METIX-BS)) were tested to evaluate PAH biodegradation in sewage sludge. In parallel, two chemical processes (quite similar Fenton processes: chemical metal leaching (METIX-AC) and chemical stabilization (STABIOX)) and one electrochemical process (electrochemical stabilization (ELECSTAB)) were tested to measure PAH removal by these oxidative processes. Moreover, PAH solubilisation from sludge by addition of a nonionic surfactant Tween 80 (Tw80) was also tested. The best yields of PAH removal were obtained by MAD and METIX-BS with more than 95% 3-ring PAH removal after a 21-day treatment period. Tw80 addition during MAD treatment increased 4-ring PAHs removal rate. In addition, more than 45% of 3-ring PAHs were removed from sludge by METIX-AC and during ELECSTAB process were quiet good with approximately 62% of 3-ring PAHs removal. However, little weaker removal of 3-ring PAHs (<35%) by STABIOX. None of the tested processes were efficient for the elimination of high molecular weight (> or = 5-ring) PAHs from sludge.     

Comparison of solid and liquid-phase bioassays using ecoscores to assess contaminated soils

Bioassays on aqueous and solid phases of contaminated soils were compared, belonging to a wide array of trophic and response levels and using ecoscores for evaluating ecotoxicological and genotoxicological endpoints. The method was applied to four coke factory soils contaminated mainly with PAHs, but also to a lesser extent by heavy metals and cyanides. Aquatic bioassays do not differ from terrestrial bioassays when scaling soils according to toxicity but they are complementary from the viewpoint of ecological relevance. Both aquatic and terrestrial endpoints are strongly correlated with concentrations of 3-ring PAHs. This evaluation procedure allows us to propose a cost-effective battery which embraces a wide array of test organisms and response levels: it includes two rapid bioassays (Microtox(?) and springtail avoidance), a micronucleus test and three bioassays of a longer duration (algal growth, lettuce germination and springtail reproduction). This battery can be recommended for a cost-effective assessment of polluted/remediated soils.     

我国环境介质中多环芳烃的分布及其生态风险

持久性有机污染物多环芳烃(PAHs)在我国环境介质中广泛分布,美国EPA规定的16种.优先控制多环芳烃大多在我国大气、水体、沉积物、土壤和生物体内检出.总结了我国环境介质中PAHs污染水平及特点,分析了其存在的环境风险.我国大气中PAHs污染较重,尤其是北方.水体已普遍受PAHs污染,其中部分水体污染严重;沉积物多环芳烃污染大多处于低生态风险水平,但沉积记录研究表明有越来越严重的趋势.我国土壤和生物体PAHs含量较低,污染生态风险较小.部分区域蔬菜中PAHs含量较高,存在不可忽视的生态风险.     

Polycyclic aromatic hydrocarbons in weathered bottom ash from incineration of municipal solid waste

Polycyclic aromatic hydrocarbons (PAHs) were analysed in weathered bottom ash from different municipal solid waste incinerators. The sum of the 16 "USEPA" PAHs was found to vary from 480 to 3590 microg/kg. The amounts of carcinogenic PAHs were between 89 and 438 microg/kg ash. The maximum levels of carcinogenic PAHs exceed the Swedish generic guidelines for sensitive land use. The results showed that the amount of PAHs in fresh and weathered bottom ash are similar, indicating that the PAHs are strongly bound to the ash and only limited amounts are released to the surroundings.     

PAHs in background soils from Western Europe: influence of atmospheric deposition and soil organic matter

The levels and distribution of polynuclear aromatic hydrocarbons (PAHs) were determined in soil samples from background locations in the UK and Norway, to investigate their spatial distribution and the controlling environmental factors. Concentrations ranged between 42 and 11200 microg kg(-1) (geometric mean 640 microg kg(-1)) and 8.6 and 1050 microg kg(-1) (150 microg kg(-1)) dry weight in the UK and Norwegian soil, respectively. Proximity to sources and locations susceptible to high atmospheric depositional inputs resulted in higher concentrations. Statistically significant relationships were observed between PAH and total organic carbon (TOC) in the Norwegian samples. High molecular weight PAHs correlated with black carbon (BC) in UK-woodland soil. These observations support the hypothesis that TOC plays an important role in the retention of PAHs in soil and that PAHs are often combined with BC during combustion emissions. PAHs with 4 and more rings comprised approximately 90% of total PAHs in the UK soil, but only 50% in the Norwegian soil. The mixture of PAHs implied that fractionation occurred during long-range atmospheric transport and deposition. The lighter PAHs with lower K(ow) values more readily reached the most remote sites. The heavier PAHs with higher K(ow) values remained in closer proximity to sources.     

Removal of polycyclic aromatic hydrocarbons from soil: a comparison between bioremoval and supercritical fluids extraction

Polycyclic aromatic hydrocarbons (PAHs) are carcinogenic substances which are resistant to environmental degradation due to their highly hydrophobic nature. Soils contaminated with PAHs pose potential risks to human and ecological health, therefore concern over their adverse effects have resulted in extensive studies on their removal from contaminated soils. The main purpose of this study was to compare experimental results of PAHs removal, from a natural certified soil polluted with PAHs, by biological methods (using bioaugmentation and biostimulation in a solid-state culture) with those from supercritical fluid extraction (SFE), using supercritical ethane as solvent. The comparison of results between the two methods showed that maximal removal of naphthalene, acenaphthene, fluorene, and chrysene was performed using bioremediation; however, for the rest of the PAHs considered (fluoranthene, pyrene, and benz(a)anthracene) SFE resulted more efficient. Although bioremediation achieved higher removal ratios for certain hydrocarbons and takes advantage of the increased rate of natural biological processes, it takes longer time (i.e. 36 d vs. half an hour) than SFE and it is best for 2-3 PAHs rings.     

Effect of a cationic surfactant on the volatilization of PAHs from soil

Purpose

Cationic surfactants are common in soils because of their use in daily cosmetic and cleaning products, and their use as a soil amendment for the mitigation and remediation of organic contaminated soils has been proposed. Such surfactant may affect the transfer and fate of organic contaminants in the environment. This study investigated the effect of a cationic surfactant, dodecylpyridinium bromide (DDPB), on the volatilization of polycyclic aromatic hydrocarbons (PAHs) from a paddy soil.

Materials and methods

The volatilization of PAHs from moist soil amended with different concentrations of DDPB was tested in an open system. The specific effects of DDPB on the liquid?Cvapor and solid?Cvapor equilibriums of PAHs were separately investigated in closed systems by headspace analysis.

Results and discussion

DDPB affects both liquid?Cvapor and solid?Cvapor processes of PAHs in soil. At DDPB concentrations below the critical micelle concentration (CMC), movement of PAHs from the bulk solution to the gas?Cliquid interface appeared to be facilitated by interaction between PAHs and the surfactant monomers adsorbed at the gas?Cliquid interface, promoting the volatilization of PAHs from solution. However, when DDPB was greater than the CMC, volatilization was inhibited due to the solubilization of PAHs by micelles. On the other hand, the formation of sorbed surfactant significantly inhibited the solid?Cvapor volatilization of PAHs.

Conclusions

The overall effect of the two simultaneous effects of DDPB on liquid?Cvapor and solid?Cvapor processes was a decreased volatilization loss of PAHs from soil. Inhibition of PAH volatilization was more significant for the soil with a lower moisture content.