首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 0 毫秒
1.
The effect of elemental carbon (EC) on global as well as regional climate forcing is potentially very important. However, the EC data for northeastern U.S. is sparse. Daily EC concentrations, [EC], and [SO4] were measured in the northeastern U.S. at a regionally representative rural site, Whiteface Mountain (WFM; 44.366°N, 73.903°W, 1.5 km amsl, above mean sea level), New York (NY), for 1997. The air mass origin was determined using 6-h backward in time air trajectories obtained from the Hybrid Single-Particle Lagrangian Integrated Trajectory Model (HYSPLIT 4). [EC] and [SO4] were highly variable and influenced by synoptic–scale meteorology (rainy vs dry periods). The maximum daily [EC] and [SO4] were 364 ± 55 and 28,800 ± 3000 ng m?3, respectively. [EC] and [SO4] also showed seasonal variations at WFM. Occurrences of high daily [EC] were mainly in spring months, while peak daily [SO4] concentrations occurred in summer months. This behavior of aerosols is due to the fact that the sources of EC and SO4 are not the same and also due to the enhanced photochemical activity during summer months that increased the production of SO4 from SO2. High [EC] and [SO4] values were associated with westerly air flow from the industrialized Midwestern U.S. Sector analysis using HYSPLIT 4 air trajectories showed that regions lying between the southwest and northwest of the WFM contributed 81% and 83% of the [EC] and [SO4], respectively. The monthly net direct radiative forcing for shortwave (SW) due to EC and SO4 aerosols at the top of the atmosphere (TOA) varied from ?0.05 to ?0.50 W m?2, with an annual average of ?0.20 ± 0.15 W m?2 that gives a net cooling effect. Average net radiative forcing at WFM for clear sky is lower than the global average radiative forcing reported by IPCC (Foster and Ramaswamy, 2007).  相似文献   

2.
Atmospheric samples of precipitation and ambient air were collected at a single site in Washington, DC, for 7 months (for ambient air samples) and 1 year (for wet deposition samples) and analyzed for arsenic, cadmium, chromium and lead. The ranges of heavy metal concentrations for 6-day wet deposition samples collected over the 1-year period were 0.20-1.3 microg/l, 0.060-5.1 microg/l, 0.062-4.6 microg/l and 0.11-3.2 microg/l for arsenic, cadmium, chromium and lead, respectively, with a precision better than 5% for more than 95% of the measurements. The ranges of heavy metal concentrations for the 6-day ambient air samples were 0.800-15.7 ng/m(3), 1.50-30.0 ng/m(3), 16.8-112 ng/m(3), and 2.90-137 ng/m(3) for arsenic, cadmium, chromium and lead, respectively, with a precision better than 10%. The spread in the heavy metal concentration over the observation period suggests a high seasonal variability for heavy metal content in both ambient air and wet deposition samples.  相似文献   

3.
Ammonia, nitric acid, sulfur dioxide and particles in two size ranges were collected at a rural site in northeastern U.S. in January–March 1984. Ammonia was collected with an oxalic acid coated denuder, all other components were collected on filters. The concentrations of ammonia ranged between 0.0 and 0.5 ppbv, nitric acid: 0.1 and 2.3 ppbv and sulfur dioxide: 1 and 52 ppbv. Ammonium and sulfate in the fine particles were highly correlated, the regression line indicated that the most abundant compound was ammonium sulphate. The content of free hydronium ions in the fine particles was well below the ammonium content. No correlation between NH3 and NH+4, HNO3 and NO3 SO3 and SO−24 could be observed.  相似文献   

4.
A unique combination of an effective sampler and analysis of individual particles has been used in studying large particles (> 5 μm) at a rural site in eastern United States. The sampler is a modified ‘high volume’ rotary inertial impactor, which consists of four collectors of different widths, rotating at high speed and collecting particles by impaction. The collector surfaces were Mylar films coated with apiezon to ensure retention. After sampling, the collection surfaces were weighted to obtain the mass-size distribution. A section of the Mylar sample was transferred to a scanning electron microscope to study in detail the morphology and elemental content of individual particles.Results from two case studies indicated the following conclusions could be made:
  • 1.(a) Natural sources, minerals and biologicals, were the main contributors to large particles (> 5 μm),
  • 2.(b) Contribution of anthropogenic sources, mainly coal-fired power plants emitting fly ash particles, was limited to a few percent of the 5–10 μm size range,
  • 3.(c) Pollen and some of the minerals were enriched in sulfur, probably as accumulation of sulfate on the particle surface,
  • 4.(d) At low wind speeds the anthropogenic contribution was enhanced, whereas at high wind speeds natural sources were almost the only contributors to the large particle mode.
In both cases the mass distribution of the large particles peaked at around 15 μm.  相似文献   

5.
Aliphatic and aromatic hydrocarbon fluxes were measured in time series sediment trap samples at 200 m and at 1000 m depths in the open Northwestern Mediterranean Sea, from December 2000 to July 2002. Averaged fluxes of n-alkanes, UCM and T-PAH35 were 2.96 ± 2.60 μg m−2 d−1, 64 ± 60 μg m−2 d−1 and 0.68 ± 0.59 μg m−2 d−1, respectively. Molecular compositions of both hydrocarbon classes showed a contamination in petrogenic hydrocarbons well above the background levels of such an open site, whereas pyrolytic hydrocarbons stand in the range of other open Mediterranean locations. Fluxes displayed ample interannual and seasonal variabilities, mainly related to mass flux variation while concentration evolutions trigger secondary changes in pollutant fluxes. High lithogenic flux events exported particles with a larger pollutant load than biogenic particles formed during the spring bloom and during the summer. Sinking hydrocarbons were efficiently transported from 200 m to 1000 m.  相似文献   

6.
In this study, we present ∼1 yr (October 1998–September 1999) of 12-hour mean ammonia (NH3), ammonium (NH4+), hydrochloric acid (HCl), chloride (Cl), nitrate (NO3), nitric acid (HNO3), nitrous acid (HONO), sulfate (SO42−), and sulfur dioxide (SO2) concentrations measured at an agricultural site in North Carolina's Coastal Plain region. Mean gas concentrations were 0.46, 1.21, 0.54, 5.55, and 4.15 μg m−3 for HCl, HNO3, HONO, NH3, and SO2, respectively. Mean aerosol concentrations were 1.44, 1.23, 0.08, and 3.37 μg m−3 for NH4+, NO3, Cl, and SO42−, respectively. Ammonia, NH4+, HNO3, and SO42− exhibit higher concentrations during the summer, while higher SO2 concentrations occur during winter. A meteorology-based multivariate regression model using temperature, wind speed, and wind direction explains 76% of the variation in 12-hour mean NH3 concentrations (n=601). Ammonia concentration increases exponentially with temperature, which explains the majority of variation (54%) in 12-hour mean NH3 concentrations. Dependence of NH3 concentration on wind direction suggests a local source influence. Ammonia accounts for >70% of NHx (NHx=NH3+NH4+) during all seasons. Ammonium nitrate and sulfate aerosol formation does not appear to be NH3 limited. Sulfate is primarily associated ammonium sulfate, rather than bisulfate, except during the winter when the ratio of NO3–NH4+ is ∼0.66. The annual average NO3–NH4+ ratio is ∼0.25.  相似文献   

7.
The ambient air in Northern Italy is characterised by relatively high PAH and PM10 concentrations in relation to calm wind and intensive temperature inversions, especially during cold periods. These stagnant conditions are occasionally interrupted by North-Föhn events, which cause a drop in relative humidity and an increase in O3 levels, indicating the mixing of local and free troposphere air flows. In this study the influence of the North-Föhn on concentrations of tracer organic compounds, including polycyclic aromatic hydrocarbons (PAHs), PM10, O3 and black carbon (BC) was studied during a North-Föhn event in November 2007. Large fluctuations in the concentration of these compounds, as well as changes in PM10 composition due to daytime and night-time variations of local source emissions were observed. Although these events occur at low frequencies (6-10%) they can for short periods, strongly affect the regional air quality by quickly decreasing the concentrations of these tracer organic compounds.  相似文献   

8.
This study compared the variations in the mass of certain particles at an urban site, Washington, DC, and at a remote site, Shenandoah National Park, VA, in the eastern United States. Seven years (1991-1997) of Interagency Monitoring of Protected Visual Environments (IMPROVE) fine particulate matter (PM2.5), PM10, coarse fraction, SO4(2-), and total sulfur data were used for this study together with available meteorology/climatology data. Various statistical modeling and analysis procedures, including time series analysis, factor analysis, and regression modeling, were employed. Time series of the constituents were divided into four terms: the long-term mean, the intraannual perturbation, the interannual perturbation, and the synoptic perturbation. PM2.5 at the two sites made up approximately 72% of the total mass for PM10, and the coarse fraction made up the remaining 28%, on average. Thirty-one percent of the PM2.5 at the DC site and 42% at the Shenandoah site was SO4(2-), based on average data for the entire period. At the DC site, the two main contributors to the constituent mass were the long-term mean and the synoptic perturbation terms, and at the Shenandoah site, they were the long-term mean and the intra-annual perturbation terms. This suggested that the constituent mass at the two sites was affected by very different processes. The terms that provided the principal contribution to the constituent mass at the two sites were studied in detail. At the DC site, dew point trends, a climate variable, were the primary driver of the 7-year trends for PM2.5, PM10, the coarse fraction, and total sulfur, and SO2 emission trends were the primary driver of the trends for SO4(2-). SO2 emission trends influenced the trends for PM2.5 and total sulfur, appearing as the second term in the model, but only parameters dealing with climate trends had significant effects on the trends for PM10 and the coarse fraction. At the Shenandoah site, only parameters dealing with climate trends affected long-term particle trends.  相似文献   

9.
The concentrations of some polycyclic aromatic hydrocarbons (PAH) and oxygenated PAH (O-PAH) can be changed by oxidation reactions during sampling. This can lead to an over- or underestimation of the corresponding adverse health effects. The aim of this study was the evaluation of these sampling artefacts. The potential of using an oxidant denuder was shown by parallel low-volume sampling with and without MnO2 ozone denuder. Twenty-three PAH and 11 O-PAH in ambient air were analysed, both in the vapour and particulate phase. The denuder was proven to be highly efficient for stripping ozone from air while causing no significant particle losses. In general, the concentrations of 5- to 7-ring PAH, which are predominantly associated with particles, were underestimated in non-denuded samples. The highest losses due to reaction with ozone and other atmospheric oxidants were observed for benzo[a]pyrene and perylene. Concurrently, the concentrations of most of the mainly particle-associated 4- to 5-ring O-PAH were higher in the non-denuded samples. The denuder did not only remove ozone, moreover other gaseous species such as more volatile PAH and O-PAH were partially oxidized on the catalytic surface, too. Degradation of PAH and concurrent degradation/formation reactions of O-PAH occurred. The corresponding reactivities of selected PAH and O-PAH are discussed.  相似文献   

10.
Ethene and formaldehyde concentrations were measured at two forest sites (valley, mountain top) in the Achen Valley (Austrian Alps, Tyrol) during three campaigns in 2001 and 2002. During the June/July campaign mean concentrations of ethene were above 9 ppbv at the valley station and 1.9 ppbv at the mountain top site; lower ethene concentrations were observed at the valley site during the April (1.4 ppbv) and the May campaign (3.1 ppbv). As 9 ppbv is the effect-related limiting value (= concentration of pollutants in the atmosphere, above which direct adverse effects on receptors may occur according to the present knowledge) of the Austrian Academy of Sciences for plants (1997) we found that ethene levels in valleys may come close to the limiting value. Formaldehyde concentrations were far below the effect-related limiting value of 16 ppbv. On the basis of the actual knowledge, ethene could be relevant as a phytotoxic component in alpine valleys.  相似文献   

11.
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   

12.
Bulk precipitation samples were collected at Montseny (Catalonia, NE Spain) from 1983 to 1994 and analysed for major cations and anions. The samples were classified for provenance based on meteorological synoptic maps and back trajectory analysis to identify the source areas of pollutants in precipitation. The meteorological classification was compared to an independent grouping based on multivariate data analysis (Clustering and Principal Component Analysis). Alkaline rain (mean pH=7.2) was associated to African trajectories. Local events produced neutral rains (mean pH=5.5). Acid rain was associated to rains of Atlantic origin (mean pH=4.8) and to European rains (mean pH=4.4), which also presented the highest mean concentrations of NH+4 (57 μeq -1), NO-3(49 μeq -1) and SO2-4(103 μeq -1). However, European events were only a small fraction of the total precipitation (10% of the cases). Marine rains accounted for 52% of the events, and African and Local for 20 and 18%, respectively. During the 11 year period there was a decreasing trend for the frequency of European events.  相似文献   

13.
Although the use of the insecticide γ-hexachlorocyclohexane (HCH) is now prohibited in many countries because of its hazardousness, stockpiles of γ-HCH still exist. In this study, we subjected γ-HCH to mechanochemical (MC) treatment with a planetary ball mill in the presence of CaO to investigate the feasibility of using this method for the treatment of γ-HCH stockpiles. We confirmed the degradation of γ-HCH and investigated the degradation mechanism. The major intermediates were identified to be 1,3,4,5,6-pentachlorocyclohexene (γ-PCCH) and chlorobenzenes (CBzs). Analysis of the steric structure of γ-HCH and identification of the degradation intermediates suggested that successive dehydrochlorination led to the formation of trichlorobenzenes. Products of further degradation (dichlorobenzenes, monochlorobenzene, and benzene) were also detected. Surprisingly, methane and ethane were also detected, which suggests cleavage of the C-C bonds of the cyclohexane ring and hydrogenation. All of the chlorine atoms in the γ-HCH could be transformed into inorganic chloride compounds by the MC treatment with CaO. Our results indicate that γ-HCH can be completely dechlorinated by MC treatment.  相似文献   

14.
An Attenuated Total Reflectance-Fourier Transform Infrared (ATR-FTIR) spectroscopic method was used to measure organic functional groups and inorganic ions at Tonto National Monument (TNM), an Interagency Monitoring of Protected Visual Environments (IMPROVE) sampling site in a rural area near Phoenix, Arizona. Functional groups and ions from common aerosol compound classes such as aliphatic and aromatic CH, methylene, methyl, aldehydes/ketones, carboxylic acids, ammonium sulfate and nitrate as well as functional groups from difficult to measure compound classes such as esters/lactones, acid anhydrides, carbohydrate hydroxyl and ethers, amino acids, and amines were quantified. On average, ~33% of the PM1.0 mass was composed of organic aerosol. The average (standard deviation) composition of the organic aerosol at TNM was 34% (6%) biogenic functional groups, 21% (5%) oxygenated functional groups, 28% (7%) aliphatic hydrocarbon functional groups (aliphatic CH, methylene and methyl) and 17% (1%) aromatic hydrocarbon functional groups. Compositional analysis, functional group correlations, and back trajectories were used to identify three types of events with source signatures: primary biogenic-influenced, urban-influenced, and regional background. The biogenic-influenced event had high concentrations of amino acids and carbohydrate hydroxyl and ether, as well as aliphatic CH and aromatic CH functional groups and qualitatively high levels of silicate. The urban-influenced events had back trajectories traveling directly from the Phoenix area and high concentrations of hydrocarbons, oxygenated functional groups, and inorganic ions. This aerosol characterization suggests that both primary emissions in Phoenix and secondary formation of aerosols from Phoenix emissions had a major impact on the aerosol composition and concentration at TNM. The regional background source had low concentrations of all functional groups, but had higher concentrations of biogenic functional groups than the urban source.  相似文献   

15.
Polycyclic aromatic hydrocarbon (PAH) concentrations have been determined for 14 successive days in a remote site of the Mediterranean Sea situated in Corsica, France. Both particulate and gas phases were collected and analyzed. For any receptor site the concentration of adsorbed PAH on particles is determined by three parameters, in order of decreasing importance: the source area, nearby sources and precipitation along the trajectory followed by the particles. For two air masses originating from the same source area, PAH concentrations can be reduced by 60% by particle scavenging during precipitation events. The identification of the source area is in complete agreement with the classification based on the mineral elements. The gas phase concentrations are determined by the source area only; they remain high compared to the concentrations in the industrial zone, thus proving that the gaseous PAH are not strongly degraded by chemical aggressors during transport. Factor analysis clearly shows the different effects involved during transport. The gas/particle ratio is determined essentially by the temperature and molecular weight of the PAH and not by the origin of the emissions. However precipitation influences this ratio to a non-negligible extent through scavenging of the aerosols. For example, the gas/particle ratio, for pyrene, varies from 2 to 4 between two ‘dry’ episodes with a temperature difference of 2.2° C, and from 6 to 13 because of the particle scavenging by rain. These results can be used as a data base and are expected to guide the conception of transport models including the parameters considered in this study.  相似文献   

16.
Passive air sampling (PAS) was employed to study the occurrence of gaseous and particle-bound PAHs in the North Chinese Plain. The averaged concentrations of gaseous and particle-bound PAHs were 485 ± 209 ng/m3 and 267 ± 161 ng/m3, respectively. The PAHs concentrations at urban sites were generally higher than those at rural ones with ratios <1.5 in spring, summer and fall, but differences between them were not significant for the wintertime and annually averaged concentrations. This urban-rural distribution pattern was related to the PAHs emission sources. PAHs spatial variation can be partially (49%) explained by emission with a simple linear regression method. Both the gaseous and particle-bound PAHs were highest in winter and lowest in summer, with winter/summer ratios of 1.8 and 8, respectively. Emission strength was the most important factor for the seasonality.  相似文献   

17.
This study investigated water-soluble ions in the sized particles (particularly nano (PM(0.01-0.056))/ultrafine (PM(0.01-0.1))) collected using MOUDI and Nano-MOUDI samplers near a busy road site and at a rural site. The analytical results demonstrate that nano and coarse particles exhibited the highest (16.3%) and lowest (8.37%) nitrate mass ratios, respectively. The mass ratio of NO(3)(-) was higher than that of SO(4)(2-) in all the sized particles at the traffic site. The secondary aerosols all displayed trimodal distributions. The aerosols in ultrafine particles collected at the roadside site exhibited Aitken mode distributions indicating they were of local origin. This finding was not observed for those ultrafine particles collected at the rural site. The mass median diameters (MMDs) of the nano, ultrafine, and fine particles were smaller at the traffic site than at the rural site, possibly related to the contribution of mobile engine emissions.  相似文献   

18.
Ground-level ozone measurements from a rural site in North-West England are presented. Two distinct types of polluted air mass are identified: one type having passed over the North Sea and Northern England, and the other having travelled from the continent via the South-East and Midlands of England. The former air mass type contains long-range transported ozone originating primarily within continental Europe, whilst the latter type contains both long-range transported ozone and ozone formed from precursors injected during passage of the air mass over middle-distance source areas in England. The monitoring results are compared with the predictions of recent theoretical models of ozone formation in polluted air masses and urban plumes.  相似文献   

19.
In a peat bog from Black Forest, Southern Germany, the rate of atmospheric Pb accumulation was quantified using a peat core dated by 210Pb and 14C. The most recent Pb accumulation rate (2.5 mg m−2 y−1) is similar to that obtained from a snowpack on the bog surface, which was sampled during the winter 2002 (1 to 4 mg m−2 y−1). The Pb accumulation rates recorded by the peat during the last 25 yr are also in agreement with published values of direct atmospheric fluxes in Black Forest. These values are 50 to 200 times greater than the “natural” average background rate of atmospheric Pb accumulation (20 μg m−2 y−1) obtained using peat samples from the same bog dating from 3300 to 1300 cal. yr B.C. The isotopic composition of Pb was measured in both the modern and ancient peat samples as well as in the snow samples, and clearly shows that recent inputs are dominated by anthropogenic Pb. The chronology and isotopic composition of atmospheric Pb accumulation recorded by the peat from the Black Forest is similar to the chronologies reported earlier using peat cores from various peat bogs as well as herbarium samples of Sphagnum and point to a common Pb source to the region for the past 150 years. In contrast, Pb contamination occurring before 1850 in southwestern Germany, differs from the record published for Switzerland mainly due to the mining activity in Black Forest. Taken together, the results show that peat cores from ombrotrophic bogs can yield accurate records of atmospheric Pb deposition, provided that the cores are carefully collected, handled, prepared, and analysed using appropriate methods.  相似文献   

20.
The Pearl River Delta (PRD) is one of the most industrialized and urbanized regions in China. With rapid growth of the economy, it is suffering from deteriorating air quality. Non-methane hydrocarbons (NMHCs) were investigated at urban and suburban sites in Guangzhou (GZ), a rural site in PRD and a clean remote site in South China, in April 2005. Additional roadside samples in GZ and Qingxi (QX, a small industrial town in PRD), ambient air samples at the rooftop of a printing factory in QX and exhaust samples from liquefied petroleum gas (LPG)—fueled taxis in GZ were collected to help identify the source signatures of NMHCs. A large fraction of propane (47%) was found in exhaust samples from LPG-fueled taxis in GZ and extremely high levels of toluene (2.0–3.1 ppmv) were found at the rooftop of the printing factory in QX. Vehicular and industrial emissions were the main sources of NMHCs. The effect of vehicular emission on the ambient air varied among the three PRD sites. The impact of industrial emissions was widespread and they contributed greatly to the high levels of aromatic hydrocarbons, especially toluene, at the three PRD sites investigated. Leakage from vehicles fueled by LPG contributed mainly to the high levels of propane and n-butane at the urban GZ site. Ethane and ethyne from long-range transport and isoprene from local biogenic emission were the main contributors to the total hydrocarbons at the remote site. Diurnal variations of NMHCs showed that the contribution from vehicular emissions varied with traffic conditions and were more influenced by fresh emissions at the urban site and by aged air at the suburban and rural sites. Isoprene from biogenic emission contributed largely to the ozone formation potential (OFP) at the remote site. Ethene, toluene and m/p-xylene were the main contributors to the OFP at the three PRD sites.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号