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1.
Fine particle (PM2.5) samples were collected, using a charcoal diffusion denuder, in two urban areas of Chile, Santiago and Temuco, during the winter and spring season of 1998. Molecular markers of the organic aerosol were determined using GC/MS. Diagnostic ratios and molecular tracers were used to investigate the origin of carbonaceous aerosols. As main sources, road and non-road engine emissions in Santiago, and wood burning in Temuco were identified. Cluster analysis was used to compare the chemical characteristics of carbonaceous aerosols between the two urban environments. Distinct differences between Santiago and Temuco samples were observed. High concentrations of isoprenoid (30–69 ng m−3) and unresolved complex mixture (UCM) of hydrocarbons (839–1369 ng m−3) were found in Santiago. High concentrations of polynuclear aromatic hydrocarbons (751±304 ng m−3) and their oxygenated derivatives (4±2 ng m−3), and of n-alk-1-enes (16±13 ng m−3) were observed in Temuco.  相似文献   

2.
Higher plant waxes are the predominant natural components in the lipid fractions (> C15) of aerosols sampled over rural and oceanic regions. Hydrocarbon, fatty acid, ketone and fatty alcohol fractions of the lipids were characterized in terms of their contents of homologous compound series and specific biogenic molecular markers. Particulate samples from the rural western United States have been analyzed and compared with samples from urban Los Angeles and remote areas over the Atlantic Ocean. The samples from rural sites contained predominantly vascular plant wax and lesser amounts of higher plant sterols and resin residues. Urban samples and, to varying degrees, some rural samples contained primarily higher weight residues of petroleum products. The loadings of hydrocarbons derived from higher plant waxes ranged approximately from 10 to 160 ng m−3 of air (for fatty acids, 10–100 ng m−3 and for fatty alcohols, 10–200 ng m−3). Higher molecular weight lipids (i.e. plant epicuticular wax, terpenes, etc.) from flora comprise a significant component of the organic carbon in rural aerosols. Primary biogenic residues are major components of aerosols in all areas and they are important components in the global cycling of organic carbon.  相似文献   

3.
PM2.5 aerosols were collected in Nanjing, a typical mega-city in China, during summer and winter 2004 and were characterized for aromatic and cyclic compounds using a GC/MS technique to understand the air pollution problem. They include polycyclic aromatic hydrocarbons (PAHs), hopanes, phthalates and hydroxy-PAHs (OH-PAHs). PAHs, hopanes and OH-PAHs presented higher concentrations in winter (26–178, 3.0–18, and 0.013–0.421 ng m−3, respectively) than in summer (12–96, 1.6–11, and 0.029–0.171 ng m−3, respectively) due to an enhanced coal burning for house heating and atmospheric inversion layers developed in the cold season. In contrast, phthalates are more abundant in summer (109–368 ng m−3, average 230 ng m−3) than in winter (33–390 ng m−3, average 170 ng m−3) due to an enhanced evaporation from plastics during the hot season and the subsequent deposition on the pre-existing particles. Generally, all the identified compounds showed higher concentrations in nighttime than in daytime due to inversion layers and increased emissions from heavy-duty trucks at night. PAHs, hopanes and phthalates in Nanjing aerosols are 5–100 times more abundant than those in Los Angeles, USA, indicating a serious air pollution problem in the city. Concentrations of OH-PAHs are 1–3 orders of magnitude less than their parent PAHs and comparable to those reported from other international cities. Source identification using diagnostic ratios of the organic tracers suggests that PAHs in Nanjing urban area are mainly derived from coal burning, whereas hopanes are more attributable to traffic emissions.  相似文献   

4.
Mercury (Hg) emissions from gasoline, diesel, and liquefied petroleum gas (LPG) vehicles were measured and speciated (particulate, oxidized, and elemental mercury). First, three different fuel types were analyzed for their original Hg contents; 571.1±4.5 ng L−1 for gasoline, 185.7±2.6 ng L−1 for diesel, and 1230.3±23.5 ng L−1 for LPG. All three vehicles were then tested at idling and driving modes. Hg in the exhaust gas was mostly in elemental form (Hg0), and no detectable levels of particulate (Hgp) or oxidized (Hg2+) mercury were measured. At idling modes, Hg concentrations in the exhaust gas of gasoline, diesel, and LPG vehicles were 1.5–9.1, 1.6–3.5, and 10.2–18.6 ng m−3, respectively. At driving modes, Hg concentrations were 3.8–16.8 ng m−3 (gasoline), 2.8–8.5 ng m−3 (diesel), and 20.0–26.9 ng m−3 (LPG). For all three vehicles, Hg concentrations at driving modes were higher than at idling modes. Furthermore, Hg emissions from LPG vehicle was highest of all three vehicle types tested, both at idling and driving modes, as expected from the fact that it had the highest original fuel Hg content.  相似文献   

5.
The concentrations and size distributions of low molecular weight dicarboxylic acids in suburban particulate matter collected in early and mid-autumn 2002 and early and mid-summer 2003 in Tainan, Taiwan, were analyzed. PM2.5 contained, on average, 449.3 ng m−3 oxalic acid, 53.0 ng m−3 malic acid, 45.5 ng m−3 maleic acid, 29.6 ng m−3 succinic acid, 20.8 ng m−3 malonic acid, and 11.6 ng m−3 tartaric acid. Bar tartaric acid, concentrations were higher during the day, indicating that these acids are photochemical products. Furthermore, the malonic acid–succinic acid ratio of 0.79 during daytime and 0.60 during nighttime demonstrates that more succinic acid is converted to malonic acid during daytime, and that aerosol dicarboxylic acids predominantly originate from photochemical oxidation during daytime. The concentration peak of oxalic acid occurred in the condensation and droplet modes (0.32–1.0 μm), as did that of sulfate. In early summer, succinic acid, malonic acid, and oxalic acid major concentration peaks occurred at 0.32–0.54 μm, indicative of the relationship created by photochemical decomposition of succinc acid into malonic acid into oxalic acid. This photochemical decomposition accelerated in mid-summer such that most concentration peaks for succinic and malonic acids also occurred at 0.32–1.0 μm. Mid-summer is also the wettest period of the four in Tainan, with 85% RH. As a result of hygroscopic reactions in mid-summer, malonic acid and oxalic acid major concentration peaks shifted from 0.32–0.54 μm or 0.54–1.0 μm to 1.0–1.8 μm, thus extending the range in which these species were found to larger particle sizes, and this shift was highly correlated with a shift in succinic acid size distribution. This latter observation offers additional evidence that succinic acid is photochemically decomposed into malonic acid and oxalic acid and that the presence of malonic and oxalic acids in the wet mid-summer atmosphere is made more obvious via hygroscopic growth. Close correlation between succinic acid and Na+ and succinic acid and NO3 in the coarse mode is related to sea spray.  相似文献   

6.
Estimates of the atmospheric deposition to Galveston Bay of polycyclic aromatic hydrocarbons (PAHs) are made using precipitation and meteorological data that were collected continuously from 2 February 1995 to 6 August 1996 at Seabrook, TX, USA. Particulate and vapor phase PAHs in ambient air and particulate and dissolved phases in rain samples were collected and analyzed. More than 95% of atmospheric PAHs were in the vapor phase and about 73% of PAHs in the rain were in the dissolved phase. Phenanthrene and napthalene were the dominant compounds in air vapor and rain dissolved phases, respectively, while 5 and 6 ring PAH were predominant in the particulate phase of both air and rain samples. Total PAH concentrations ranged from 4 to 161 ng m−3 in air samples and from 50 to 312 ng l−1 in rain samples. Temporal variability in total PAH air concentrations were observed, with lower concentrations in the spring and fall (4–34 ng m −3) compared to the summer and winter (37–161 ng m−3). PAHs in the air near Galveston Bay are derived from both combustion and petroleum vaporization. Gas exchange from the atmosphere to the surface water is estimated to be the major deposition process for PAHs (1211 μg m− 2 yr− 1), relative to wet deposition (130 μg m−2 yr− 1) and dry deposition (99 μg m−2 yr− 1). Annual deposition of PAHs directly to Galveston Bay from the atmosphere is estimated as 2  t yr−1.  相似文献   

7.
Trace elements and metals in the ultrafine (<0.18 μm) and accumulation (0.18–2.5 μm) particulate matter (PM) modes were measured during the winter season, next to a busy Southern California freeway with significant (∼20%) diesel traffic. Both ambient and concentrated size-segregated impactor samples were taken in order to collect enough mass for chemical analysis. Data at this location were compared to a site located 1 mile downwind of the freeway, which was reflective of urban background. The most abundant trace elements in the accumulation mode detected by inductively coupled plasma mass spectroscopy (ICPMS) were S (138 ng m−3), Na (129 ng m−3), and Fe (89 ng m−3) while S (35 ng m−3) and Fe (35 ng m−3) were the most abundant in the ultrafine mode. The concentrations of several trace elements, including Mg, Al, and Zn, and in particular Ca, Cu, and Pb, did not uniformly increase with size within fine PM, an indication that various roadway sources exist for these elements. Calculation of crustal enrichment factors for the two sites indicates that the freeway traffic contributed to enriched levels of ultrafine Cu, Ba, P and Fe and possibly Ca. The results of this study show that trace elements constitute a small fraction of PM mass in the nanoparticle size range, but these can and should be characterized due to their likely importance to human health.  相似文献   

8.
The aerosol scattering properties were investigated at two continental sites in northern China in 2004. Aerosol light scattering coefficient (σsp) at 525 nm, PM10, and aerosol mass scattering efficiencies (α) at Dunhuang had a mean value of 165.1±148.8 M m−1, 157.6±270.0 μg m−3, and 2.30±3.41 m2 g−1, respectively, while these values at Dongsheng were, respectively, 180.2±151.9 M m−1, 119.0±112.9 μg m−3, and 1.87±1.41 m2 g−1. There existed a seasonal variability of aerosol scattering properties. In spring, at Dunhuang PM10, σsp, and α were 184.1±211.548 μg m−3, 126.3±89.6 M m−1, and 1.05±0.97 m2 g−1, respectively, and these values at Dongsheng were 146.4±142.1 μg m−3, 183.4±81.7 M m−1, and 1.98±1.52 m2 g−1, respectively. However, in winter at Dunhuang PM10, σsp, and α were 158.1±261.4 μg m−3, 303.3±165.2 M m−1, and 3.17±1.93 m2 g−1, respectively, and these values at Dongsheng were 155.7±170.1 μg m−3, 304.4±158.1 M m−1, and 2.90±1.72 m2 g−1, respectively. σsp and α in winter were higher than that in spring at both the sites, which coincides with the characteristics of dust aerosol and pollution aerosol. Overall, the dominant aerosol types in spring and winter at both sites in northern China are dust aerosol and pollution aerosol, respectively.  相似文献   

9.
Micrometeorological measurements and ambient air samples, analyzed for concentrations of NH3, HNO3, NH4+, and NO3, were collected at an alpine tundra site on Niwot Ridge, Colorado. The measured concentrations were extremely low and ranged between 5 and 70 ng N m−3. Dry deposition fluxes of these atmospheric species were calculated using the micrometeorological gradient method. The calculated mean flux for NH3 indicates a net deposition to the surface and indicates that NH3 contributed significantly to the total N deposition to the tundra during the August–September measurement period. Our pre-measurement estimate of the compensation point for NH3 in air above the tundra was 100–200 ng N m−3; thus, a net emission of NH3 was expected given the low ambient concentrations of NH3 observed. Based on our results, however, the NH3 compensation point at this alpine tundra site appears to have been at or below about 20 ng N m−3. Large deposition velocities (>2 cm s−1) were determined for nitrate and ammonium and may result from reactions with surface-derived aerosols.  相似文献   

10.
The tests of standard mixtures and four sets of atmospheric particulate samples showed that an acid-wash (AW) pretreatment of fluorocarbon-coated glass fiber filters prior to aerosol sampling enhanced the quantifiable organic compounds for more than 29% (or 66 ng m−3); in particular, 47–273 ng m−3 (21–366%) more water-soluble organic compounds (WSOCs) were measured. When the acid-pretreated filters were employed, up to nine more organic species were measured in the individual daily samples. Because the acid pretreatment reduced the metal contaminants in the glass fiber filters, using the AW filters for aerosol sampling allows higher extraction recoveries of organic compounds. Since the fingerprinting compounds were more accurately determined when the aerosol samples were collected on the AW filters, better assessment of emission sources and toxicity of air pollutants can be obtained.  相似文献   

11.
The effect of black carbon (BC) on climate forcing is potentially important, but its estimates have large uncertainties due to a lack of sufficient observational data. The BC mass concentration in the southeastern US was measured at a regionally representative site, Mount Gibbes (35.78°N, 82.29°W, 2006 m MSL). The air mass origin was determined using 48-h back trajectories obtained from the hybrid single-particle Lagrangian integrated trajectory model. The highest average concentration is seen in polluted continental air masses and the lowest in marine air masses. During the winter, the overall average BC value was 74.1 ng m−3, whereas the overall summer mean BC value is higher by a factor of 3. The main reason for the seasonal difference may be enhanced thermal convection during summer, which increases transport of air pollutants from the planetary boundary layer of the surrounding urban area to this rural site. In the spring of 1998, abnormally high BC concentrations from the continental sector were measured. These concentrations were originating from a biomass burning plume in Mexico. This was confirmed by the observations of the Earth probe total ozone mapping spectrometer. The BC average concentrations of air masses transported from the polluted continental sector during summer are low on Sunday to Tuesday with a minimum value of 256 ng m−3 occurring on Monday, and high on Wednesday to Friday with a maximum value of 379 ng m−3 occurring on Friday. The net aerosol radiative forcing (scattering effects plus absorption effects) per unit vertical depth at 2006 m MSL is calculated to be −1.38×10−3 W m−3 for the southeastern US. The magnitude of direct radiative forcing by aerosol scattering is reduced by 15±7% due to the BC absorption.  相似文献   

12.
Five weeks of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle bound mercury (Hgp) concentrations as well as fluxes of GEM were measured at Maryhill, Ontario, Canada above a biosolids amended field. The study occurred during the autumn of 2004 (October–November) to capture the effects of cool weather conditions on the behaviour of mercury in the atmosphere. The initial concentration of total mercury (Hg) in the amended soil was relatively low (0.4 μg g−1±10%).A micrometeorological approach was used to infer the flux of GEM using a continuous two-level sampling system with inlets at 0.40 and 1.25 m above the soil surface to measure the GEM concentration gradient. The required turbulent transfer coefficients were derived from meteorological parameters measured on site. The average GEM flux over the study was 0.1±0.2 ng m−2 h−1(±one standard deviation). The highest averaged hourly GEM fluxes occurred when the averaged net radiation was highest, although the slight diurnal patterns observed were not statistically significant for the complete flux data series. GEM emission fluxes responded to various local events including the passage of a cold front when the flux increased to 2 ng m−2 h−1 and during a biosolids application event at an adjacent field when depositional fluxes peaked at −3 ng m−2 h−1. Three substantial rain events during the study kept the surface soil moisture near field capacity and only slightly increased the GEM flux. Average concentrations of RGM (2.3±3.0 pg m−3), Hgp (3.0±6.2 pg m−3) and GEM (1.8±0.2 ng m−3) remained relatively constant throughout the study except when specific local events resulted in elevated concentrations. The application of biosolids to an adjacent field produced large increases in Hgp (25.8 pg m−3) and RGM (21.7 pg m−3) concentrations only when the wind aligned to impact the experimental equipment. Harvest events (corn) in adjacent fields also corresponded to higher concentrations of GEM and Hgp but with no elevated peaks in RGM concentrations. Diurnal patterns were not statistically significant for RGM and Hgp at Maryhill.  相似文献   

13.
14.
PM10 aerosols at McMurdo Station, Antarctica were sampled continuously during the austral summers of 1995–1996 and 1996–1997. PM10 (particles with aerodynamic diameters less than 10 μm) mass concentrations at Hut Point, located less than 1 km from downtown McMurdo, averaged 3.4 μg m−3, more than an order of magnitude lower than the USEPA annual average National Ambient Air Quality Standard (NAAQS) of 50 μg m−3. Concentrations of methanesulfonate and nitrate were similar to those measured at other Antarctic coastal sites. Non-sea-salt sulfate (NSS) concentrations on Ross Island were higher than those found at other coastal locations. The average elemental carbon concentration (129 ng m−3) downwind of the station was two orders of magnitude higher than those measured at remote coastal and inland Antarctic sites during summer. Average sulfur dioxide concentrations (746 ng m−3) were 3–44 times higher than those reported for coastal Antarctica. Concentrations of Pb and Zn were 17 and 46 times higher than those reported for the South Pole. A methanesulfonate to biogenic sulfate ratio (R) of 0.47 was derived that is consistent with the proposed temperature dependence of R.  相似文献   

15.
Filters collected from the Southeastern Aerosol Research and Characterization (SEARCH) air monitoring network were analyzed for the presence of 2-methyltetrols, namely 2-methylthreitol and 2-methylerythritol, two compounds that are products of the photooxidation of isoprene and have been detected in aerosol at a variety of sites around the globe. The 2-methytetrols were detected in ambient filter samples collected at the four SEARCH sites, Birmingham, AL, Centreville, AL, Pensacola, FL, and at Jefferson Street in Atlanta, GA, in late June 2004. Average atmospheric concentrations of 11.9 and 4.8 ng m−3 were measured for 2-methylerythritol and 2-methylthreitol, respectively, at the inland sampling sites, whereas average concentrations of 4.9 and 1.6 ng m−3 were measured at the coastal sampling location (Pensacola). On average, the aerosol loading from these two compounds accounts for approximately 0.42% and 0.21% of the organic mass collected on a given sampling day at the inland and coastal sites, respectively. The present data on these compounds, which are particulate-phase fingerprints of isoprene photooxidation, add to the growing body of ambient data on secondary organic aerosol from isoprene.  相似文献   

16.
The gas phosphine (PH3) is a part of an atmospheric link of the phosphorus cycle on earth. Previous research reported the terrestrial lower tropospheric PH3 at night in the 1 ng m−3 range in remote areas, with the peak of 100 ng m−3 in populated areas, and at daytime even lower concentrations in the pg m−3 range. The data of the global marine atmospheric PH3 are still very sparse.This study presents surprisingly high concentrations of PH3 in the order of 0.1–1 μg m−3 in many of 32 samples of the marine atmosphere in the latitudinal range from 30°N to 65°S (the cruise of research ship Xuelong from Shanghai Harbor, China, to Antarctica). The highest concentrations were measured near coastal areas of Eastern Asia and Western Australia. A significant correlation exists between marine atmospheric PH3 concentration and air temperature at 22:00 (local time). PH3 concentrations at different latitudes strongly decline with daylight intensity according to a logarithmic relationship. These surprisingly high concentrations of the readily oxidizable PH3 in the air indicate hitherto unknown but important PH3 emission sources in marine environment. More work is necessary to evaluate the sources of atmospheric PH3 from marine biosphere.  相似文献   

17.
Concentrations of different species of mercury in arctic air and precipitation have been measured at Ny-Ålesund (Svalbard) and Pallas (Finland) during 1996–1997. Typical concentrations for vapour phase mercury measured at the two stations were in the range of 0.7–2 ng m−3 whereas particulate mercury concentrations were below 5 pg m−3. Total mercury in precipitation was in the range 3–30 ng l−1. In order to evaluate the transport and deposition of mercury to the arctic from European anthropogenic sources, the Eulerian transport model HMET has been modified and extended to also include mercury species. A scheme for chemical conversion of elemental mercury to other species of mercury and deposition characteristics of different mercury species have been included in the model. European emission inventories for three different forms of Hg (Hg0, HgCl2 and Hgp) have been implemented in the numerical grid system for the HMET model.  相似文献   

18.
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   

19.
Marine background levels of non-sea-salt- (nss-) SO42− (5.0–9.7 neq m−3), NH4+ (2.1–4.4 neq m−3) and elemental carbon (EC) (40–80 ngC m−3) in aerosol samples were measured over the equatorial and South Pacific during a cruise by the R/V Hakuho-maru from November 2001 to March 2002. High concentrations of nss-SO42− (47–94 neq m−3), NH4+ (35–94 neq m−3) and EC (130–460 ngC m−3) were found in the western North Pacific near the coast of the Asian continent under the influence of the Asian winter monsoon. Particle size distributions of ionic components showed that the equivalent concentrations of nss-SO42− were balanced with those of NH4+ in the size range of 0.06<D<0.22 μm, whereas the concentration ratios of NH4+ to nss-SO42− in the size range of D>0.22 μm were decreased with increase in particle size. We estimated the source contributions of those aerosol components in the marine background air over the equatorial and South Pacific. Biomass burning accounted for the large fraction (80–98% in weight) of EC and the minor fraction (2–4% in weight) of nss-SO42−. Marine biogenic source accounted for several tens percents of NH4+ and nss-SO42−. In the accumulation mode, 70% of particle number existed in the size range of 0.1<D<0.2 μm. In the size rage of 0.06<D<0.22 μm, the dominant aerosol component of (NH4)2SO4 would be mainly derived from the marine biogenic sources.  相似文献   

20.
Size-fractionated particles were collected at two sites from July 2004 to April 2006 in Shanghai. The mercury in particles was extracted and divided operationally into four species: exchangeable particulate mercury (EXPM), HCl-soluble particulate mercury (HPM), elemental particulate mercury (EPM) and residual particulate mercury. The total particulate Hg concentration during the study period ranged from 0.07 ng m?3 to 1.45 ng m?3 with the average 0.56 ± 0.22 ng m?3 at site 1, while 0.20 ng m?3–0.47 ng m?3 with the average 0.33 ± 0.09 ng m?3 at site 2, which is far higher than some foreign cities and comparable to some cities with heavy air pollution in China. The Hg mass content also displayed evident size distribution, with higher value in PM1.6–3.7, somewhat higher or lower than the source profile. EXAM was only found in the summer, HPM have higher percentage in summer and fall rather than in winter and spring. The different mercury species showed different correlation to temperature, relative humidity, wind speed. HPM positively depends on temperature at both sites which implies the importance of mercury transformation on particles. In foggy days TPM increased greatly, but HPM didn't vary greatly as anticipated. Instead, RPM gained a distinguished increase. It demonstrated that aqueous reaction and complex heterogenic reactions in droplet might happen in acidic environment. The correlation of mercury with other pollutants including SO2, NO2, CO and PM10 varies with the different mercury forms. Hybrid single-particle lagrangian integrated trajectories (HYSPLIT) model was used to back trace air mass at different representative days and results indicated that transportation from Huabei Plain will increase mercury concentration in winter and fall to some extent. The possible existing compounds and their atmospheric behavior of HPM, EPM and RPM were calculated and the compared to analyze its implication on atmospheric mercury cycle.  相似文献   

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