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1.
Airborne particulate matter in Saxony (Germany) was investigated at three different sites (central urban, urban outskirts, rural) during a winter (1999/2000) and a summer (2000) campaign. PM was collected simultaneously at all three sites using five-stage Berner impactors. Besides size-segregated chemical particle characterisation and mass closure source apportionment of the particle components, especially of the carbonaceous fraction was an aim of the study. Source apportionment was performed exclusively on the basis of experimental data without support of models considering a set of basic assumptions and logical deductions. The derived simple equations permit to differentiate the carbonaceous fraction in traffic, domestic heating (winter) and biogenic (summer) contributions.The total carbon (TC) in the smallest particle size range (Dpaer = 0.05-0.14μm) at the urban site, contributing 88% to the mass in that class, was completely attributed to traffic emissions. For the particle size range Dpaer = 0.42-1.2 μm (50-60% of the total mass) TC was attributed to traffic (67%) and domestic heating (33%) in winter and to traffic (82%) and biogenic origin (18%) in summer.Size-segregated determination of alkanes revealed that these compounds were mainly of biogenic origin in summer and of anthropogenic origin in winter considering the carbon preference index (CPIodd). Particulate PAHs found in winter samples originated mainly from domestic heating and not from traffic emissions.The method described cannot provide complete results, but the demonstrated source apportionment can be helpful to assess a given situation with regard to possible steps against the exceeding of the EU limit of the PM10 mass concentration of 50 μg m−3.  相似文献   

2.
The contribution of emissions from agricultural facilities is rapidly becoming a major concern for local and regional air quality. Characterization of particle properties such as physical size distribution and chemical composition can be valuable in understanding the processes contributing to emissions and ultimate fate of particulate matter from agricultural facilities. A measurement campaign was conducted at an Iowa, deep-pit, three-barn swine finishing facility to characterize near-source ambient particulate matter. Size-specific mass concentrations were determined using minivol samplers, with additional size distribution information obtain using optical particle counters. Particulate composition was determined via ion chromatographic analysis of the collected filters. A thermal-CO2 elemental/organic carbon analyzer measured particulate carbon. The chemical composition and size distribution of sub-micron particles were determined via real-time aerosol mass spectrometry. Primary particulate was not found to be a major emission from the examined facility, with filter-based impactor samples showing average near-source increases (~15–50 m) in ambient PM10 of 5.8 ± 2.9 μg m−3 above background levels. PM2.5 also showed contribution attributable to the facility (1.7 ± 1.1 μg m−3). Optical particle counter analysis of the numerical size distributions showed bimodal distributions for both the upwind and downwind conditions, with maximums around 2.5 μm and below the minimum quantified diameter of 0.3 μm. The distributions showed increased numbers of coarse particles (PM10) during periods when wind transport came from the barns, but the differences were not statistically significant at the 95% confidence level. The PM10 aerosols showed statistically increased concentrations of sulfate, nitrate, ammonium, calcium, organic carbon, and elemental carbon when the samplers were downwind from the pig barns. Organic carbon was the major constituent of the barn-impacted particulate matter in both sub-micron (54%) and coarse size (20%) ranges. The AMS PM1 chemical speciation showed similar species increases, with the exception of and Ca+2, the latter not quantified by the AMS.  相似文献   

3.
Aerosol and rain samples were collected between 48°N and 55°S during the KH-08-2 and MR08-06 cruises conducted over the North and South Pacific Ocean in 2008 and 2009, to estimate dry and wet deposition fluxes of atmospheric inorganic nitrogen (N). Inorganic N in aerosols was composed of ~68% NH4+ and ~32% NO3– (median values for all data), with ~81% and ~45% of each species being present on fine mode aerosol, respectively. Concentrations of NH4+ and NO3− in rainwater ranged from 1.7–55 μmol L−1 and 0.16–18 μmol L−1, respectively, accounting for ~87% by NH4+ and ~13% by NO3− of total inorganic N (median values for all data). A significant correlation (r = 0.74, p < 0.05, n = 10) between NH4+ and methanesulfonic acid (MSA) was found in rainwater samples collected over the South Pacific, whereas no significant correlations were found between NH4+ and MSA in rainwater collected over the subarctic (r = 0.42, p > 0.1, n = 6) and subtropical (r = 0.33, p > 0.5, n = 6) western North Pacific, suggesting that emissions of ammonia (NH3) by marine biological activity from the ocean could become a significant source of NH4+ over the South Pacific. While NO3− was the dominant inorganic N species in dry deposition, inorganic N supplied to surface waters by wet deposition was predominantly by NH4+ (42–99% of the wet deposition fluxes for total inorganic N). We estimated mean total (dry + wet) deposition fluxes of atmospheric total inorganic N in the Pacific Ocean to be 32–64 μmol m−2 d−1, with 66–99% of this by wet deposition, indicating that wet deposition plays a more important role in the supply of atmospheric inorganic N than dry deposition.  相似文献   

4.
The concentration, radiocarbon (14C) and stable isotope (13C and 18O) content of CO have been determined in air samples collected across Russia (about 8,500 km) and along the Ob river during the summer of 1999 to study the CO sources and sinks. An instrumented carriage on the Trans-Siberian railway and a boat on the river Ob were used as atmospheric measurement platforms. In general, CO mixing ratios, CO stable isotope ratios, as well as the abundances of 14CO over West Siberia were similar to those found at remote northern hemispheric baseline monitoring stations. Identified sources of CO along the Ob appear to be connected to methane oxidation based on an inferred δ13Csource = −36.8 ± 0.6‰, while the value for δ18Osource = 9.0 ± 1.6‰ identifies it as burning. Thus flaring in the oil and gas production can be supposed to be a source. The extreme 13C depletion and concomitant 18O enrichment for two of the boat samples unambiguously indicates contamination by CO from combustion of natural gas (inferred values δ13Csource = −40.3‰ and δ18Osource = 17.5‰). For these two samples, that have strongly elevated 14CO concentrations, the industrial area near Tomsk is identified as a source area using meteorological calculations. Along the Trans-Siberian Railroad background CO was to various degrees contaminated with CO from methane combustion (δ13Csource = −35.7 ± 6.2‰ and δ18Osource = 10.3 ± 1.8‰). The impact of industrial burning was discernable in the vicinity of Perm-Kungur.  相似文献   

5.
Both aerosol and rainwater samples were collected and analyzed for ionic species at a coastal site in Southeast Asia over a period of 9 months (January–September 2006) covering different monsoons. In general, the occurrence and distribution of ionic species showed a distinct seasonal variation in response to changes in air mass origins. Real-time physical characterization of aerosol particles during rain events showed changes in particle number distributions which were used to assess particle removal processes associated with precipitation, or scavenging. The mean scavenging coefficients for particles in the range 10–500 nm and 500–10 μm were 7.0 × 10−5 ± 2.8 × 10−5 s−1 and 1.9 × 10−4 ± 1.6 × 10−5 s−1, respectively. A critical analysis of the scavenging coefficients obtained from this study suggested that the wet removal of aerosol particles was greatly influenced by rain intensity, and was particle size-dependent as well. The scavenging ratios, another parameter used to characterize particle removal processes by precipitation, for NH4 +, Cl−, SO4 2−, and NO3 − were found to be higher than those of Na+, K+, and Ca2+ of oceanic and crustal origins. This enrichment implied that gaseous species NH3, HCl, and HNO3 could also be washed out readily. These additional sources of ions in precipitation presumably counter-balanced the dilution effect caused by high total precipitation volume in the marine and tropical area.  相似文献   

6.
The paper presents the importance of the Nocturnal Boundary Layer in driving the diurnal variability of the atmospheric CO2 mixing ratio and the carbon isotope ratio at ground level from an urban station in India. Our observations are the first of their kind from this region. The atmospheric CO2 mixing ratio and the carbon isotopic ratio were measured for both the morning (05:30–07:30 IST) and afternoon time (16:00–18:00 IST) air samples at 5 m above ground level in Bangalore city, Karnataka State (12° 58′ N, 77° 38′ E, masl = 920 m) for a 10 day period during the winter of 2008. We observed a change of ~7% the in CO2 mixing ratio between the morning and afternoon time air samples. A stable isotope analysis of CO2 from morning samples showed a depletion in the carbon isotope ratio by ~2‰ compared to the afternoon samples. Along with the ground-based measurement of air samples, data of radiosonde measurements were also obtained from the Indian Meteorological Department to identify the vertical atmospheric structure at different time in a day. We proposed the presence or absence of the NBL as a controlling factor for the observed variability in the mixing ratio as well as its isotopic composition. Here we used the Keeling model approach to find out the carbon isotope ratio for the local sources. The local sources have further been characterized as anthropogenic and biological respiration (in %) using a two-component mixing model. We also used a vertical mixing model based on the concept of the mixing of isotopically depleted (carbon isotope) “polluted air” (PA) with isotopically enriched “free atmospheric air” (FA) above. Using this modeling approach, the contribution of FA at ground level is being estimated for both the morning and afternoon time air samples.  相似文献   

7.
The uptake of water vapor on MgCl2×6H2O and NaCl salt dry solid films was studied over the temperature range 240 to 340 K and at 1 Torr pressure of helium using a flow reactor coupled to a modulated molecular beam mass spectrometer. The H2O to salt uptake data were obtained from the kinetics of H2O loss on salt coated Pyrex rods. The following Arrhenius expression was obtained for the initial uptake coefficient of H2O on MgCl2×6H2O films: γ 0 (MgCl2) = (6.5 ± 1.0) × 10−6 exp[(470 ± 40)/T] (calculated with specific BET surface area, quoted uncertainties are 1σ statistical). The rate of H2O adsorption on NaCl was found to be much lower than on MgCl2×6H2O, and only an upper limit was determined for the corresponding uptake coefficient: γ (NaCl) ≤ 5.6 × 10−6 at T = 300 K. The results show that the rate of H2O adsorption to salt surfaces is drastically dependent on the salt sample composition.  相似文献   

8.
The carbon kinetic isotope effects (KIEs) in the reactions of several unsaturated hydrocarbons with chlorine atoms were measured at room temperature and ambient pressure using gas chromatography combustion isotope ratio mass spectrometry (GCC-IRMS). All measured KIEs, defined as the ratio of the rate constants for the unlabeled and labeled hydrocarbon reaction k 12/k 13, are greater than unity or normal KIEs. The KIEs, reported in per mil according to Cl ɛ = (k 12/k 13−1) × 1000‰ with the number of experimental determinations in parenthesis, are as follows: ethene, 5.65 ± 0.34 (1); propene, 5.56 ± 0.18 (2); 1-butene, 5.93 ± 1.16 (1); 1-pentene, 4.86 ± 0.63 (1); cyclopentene, 3.75 ± 0.14 (1); toluene, 2.89 ± 0.31 (2); ethylbenzene, 2.17 ± 0.17 (2); o-xylene, 1.85 ± 0.54 (2). To our knowledge, these are the first reported KIE measurements for reactions of unsaturated NMHC with Cl atoms. Relative rate constants were determined concurrently to the KIE measurements. For the reactions of cyclopentene and ethylbenzene with Cl atoms, no rate constant has been reported in refereed literature. Our measured rate constants are: cyclopentene (7.32 ± 0.88) relative to propene (2.68 ± 0.32); ethylbenzene (1.15 ± 0.04) relative to o-xylene (1.35 ± 0.21), all × 10−10 cm3 molecule−1 s−1. The KIEs in reactions of aromatic hydrocarbons with Cl atoms are similar to previously reported KIEs in Cl-reactions of alkanes with the same numbers of carbon atoms. Unlike the KIEs for previously studied gas-phase hydrocarbon reactions, the KIEs for alkene–Cl reactions do not exhibit a simple inverse dependence on carbon number. This can be explained by competing contributions of normal and inverse isotope effects of individual steps in the reaction mechanism. Implications for the symmetries of the transition state structures in these reactions and the potential relevance of Cl-atom reactions on stable carbon isotope ratios of atmospheric NMHC are discussed.  相似文献   

9.
The atmospheric processing by ozone of peptide-containing mixed particles was investigated as proxies for biogenic and sea spray primary organic aerosol. Reactions were performed in a flow reactor and particle composition was monitored by photoelectron resonance capture ionization aerosol mass spectrometry. Mixed particles containing dipeptides in a saturated organic matrix of stearic and palmitic acids showed no reaction under ozonolysis at exposure levels of 2.5 × 10−4 atm s O3. However reactions of mixed particles of a dipeptide (Leu-Leu) in an unsaturated matrix (oleic acid) under the same conditions resulted in a rapid loss of the peptide ion signal, as well as the carrier matrix, and appearance of a number of ion signals corresponding to secondary products. High molecular weight imides and amides have been identified corresponding to possible reactions of ozonolysis products and reactive intermediates (i.e. aldehydes, stabilized Criegee intermediates). Additionally, tautomerisation of the imides to enamines in the particle phase is postulated, with ozonolysis of the enamine followed by regioselective decomposition of the primary ozonide to form an amide whereby the peptide incorporates an aldehydic group at the N-terminus. The same general reactivity pattern was observed for mixed particles of diglycine and oleic acid. This behavior was not observed in solution phase experiments, where the tautomerisation favors the more stable imine form, indicating that particulate phase reactions of this nature may be dependent on the specific particle physical properties. The implications of this chemistry with respect the atmospheric aging of cell-derived organic aerosol are discussed.  相似文献   

10.
Concentrations of manganese in 56 rain events in Wilmington, NC, USA rainwater from April 1, 2005 to March 31, 2006 were 11 ± 3 nM for dissolved Mn and 1.2 ± 0.4 nM for particulate Mn. Concentrations of both forms of Mn were higher in terrestrial storms relative to marine events. This observation along with the positive correlation of Mn with pollutant indicators suggests anthropogenic inputs to rain at this location, as has been observed at other locations. The ratio of Mnpart/Mndiss was threefold larger in summer relative to winter rain, which matched the increase of particulate to dissolved Fe in rainwater suggesting influence of Saharan dust during the summer. Like Fe in rain, Mn undergoes photoreduction in rainwater, which has also been shown to be important in Mn cycling in seawater. The flux of Mn removed from the atmosphere via wet deposition is 1.5 × 10−5 moles m−2 yr−1 at this location, which is approximately twice the flux reported from two rainwater studies conducted in the early 1980s on Bermuda. Atmospheric input of Mn to the oceans is important because Mn like Fe is an essential and potentially limiting nutrient. Experiments mixing authentic rainwater and seawater demonstrate that rainwater dissolved Mn does not rapidly precipitate in seawater suggesting wet deposition is an important source of soluble, stable Mn to surface seawater.  相似文献   

11.
Functional relationships linking at λ0=351 nm aerosol extinction αλ0aer and backscatter coefficient βλ0aer of maritime and desert type aerosols are determined to allow for inversion of the single-wavelength lidar signals. Such relationships are derived as mean behavior of 20,000 extinction versus backscatter computations, performed for aerosol size distributions and compositions whose describing parameters are randomly chosen within the naturally observed variability. For desert-type aerosols, the effect of the particle non-sphericity is considered and it is shown that the extinction to backscatter ratio of non-spherical dust particles can be up to 60% larger than the values obtained for spherical particles. Aerosol extinction and backscatter coefficient profiles obtained inverting the single-wavelength lidar signal with the modeled relationships are then compared to the same profiles measured by a combined elastic-Raman lidar operating at 351 nm. Analytical back trajectories and satellite images are used to characterize advection patterns during lidar measurements and to properly choose the modeled functional relationship. A good accordance between the two techniques is found for advection patterns over the lidar site typical of maritime and dust conditions. Maximum differences between the model-based αλ0aer and βλ0aer vertical profiles and the corresponding ones measured by the combined elastic-Raman lidar technique are of 30% and 40% in maritime and desert dust conditions, respectively. The comparison of elastic-Raman lidar measurements and model-based results also reveals that particle non-sphericity must be taken into account when mineral dust-type aerosols are directly advected over the measurement site.  相似文献   

12.
Samples of airborne PM2.5 particles in Guangzhou urban area were collected during the autumn of 2006 and the spring of 2007. The morphologies and elemental compositions of individual particles were determined by Scanning Electron Microscopy coupled with Energy Dispersive X-ray Spectrometer (SEM-EDX). The obtained images were further analyzed for size distribution by an image analysis system. Based on the morphology, particles in PM2.5 were classified into four groups: soot aggregates, minerals, fly ash and others. The amount of soot aggregates and minerals were higher than that of fly ashes. The distributions of particles by number and size in two seasons were bimodal with 90% less than 1.0 μm in diameter. The primary peak from the autumn samples was in the size range of 0.4 ~ 0.5 μm, and 0.3 ~ 0.4 μm for the spring samples. More soot aggregates (36.1%) and minerals (61.5%) were found than fly ash (2.4%) in autumn, but soot aggregates (89.9%) was the dominant particle type in spring. The size distribution of particles according to the volume was generally opposite to that according to the number. Particles less than 1.0 μm were as high as 89.5% in number but contributed only 18.9% in volume, indicating that fine particles contributed relatively little in volume although existing in large numbers.  相似文献   

13.
The kinetics of heterogeneous reactions of NO2 with 17 polycyclic aromatic hydrocarbons (PAHs) adsorbed on laboratory generated kerosene soot surface was studied over the temperature range (255–330) K in a low pressure flow reactor combined with an electron-impact mass spectrometer. The kinetics of soot-bound PAH consumption due to their desorption and reaction with NO2 were monitored using off-line HPLC measurements of their concentrations in soot samples as a function of reaction time, NO2 concentrations in the gas phase being analyzed by mass spectrometer. No measurable decay of PAHs due to the reaction with NO2 was observed under experimental conditions of the study (maximum NO2 concentration of 5.5 × 1014 molecule cm−3 and reaction time of 45 min), which allowed to determine the upper limits of the first-order rate constants for the heterogeneous reactions of 17 soot-bound PAHs with NO2: k < 5.0 × 10−5 s−1 (for most PAHs studied). Comparison of these results to previous studies carried on different carbonaceous substrates, showed that heterogeneous reactivity of PAHs towards NO2 is, probably, dependent on the substrate nature even for resembling, although different carbonaceous materials. Results show that particulate PAHs degradation by NO2 alone is of minor importance in the atmosphere  相似文献   

14.
Summary In this study an attempt is made to examine and analyse the mean characteristics of the katabatic flows at the western slope foot of a 1024 m high knife edge mountain using a meteorological tower and three surface meteorological stations. In addition, the frequency distribution of the occurrence of the katabatic flow over one year period is studied along the characteristics of the flow arriving in the neighbouring urban area at a distance of 1.5 km. It was found that the katabatic flow occurs mainly in autumn and spring with the highest frequency in April. The flow is generally characterised by small depth as it is affected substantially by the background flow. The expected direction of the katabatic wind dominates mainly at the level of 7 m, where the influence of the background flow is minimised. At the level of 18 m the wind direction shifts, due to the interaction of the katabatic wind with the background flow. The katabatic flow can penetrate at a distance of 1.5 km being substantially weakened. Received September 18, 1996 Revised August 4, 1997  相似文献   

15.
Summary Latitude-altitude structure of ozone QBO over the tropical-subtropical stratosphere (40° S–40° N) has been explored by analyzing Microwave Limb Sounder (MLS) aboard Upper Atmospheric Research Satellite (UARS) data for the period 1992–1999 using the multifunctional regression model. The inferred ozone QBO shows two maxima located at 22 hPa and 10 hPa with coefficient of 2–3% per 10 m/s centered at the equator. The equatorial maxima are out of phase with each other. Subtropics exhibit two peak structure near 14 hPa but of opposite sign to that of equatorial maximum near 10 hPa. Over the equatorial region, positive (zonal winds westerly) coefficients overlay negative (zonal winds easterlies) coefficients which descend with time. A pattern of equatorial maximum and two subtropical minima appears in the months December to February near 10 hpa and it propagates upward with progression of seasons. Equatorial QBO is seasonally asynchronous while subtropical QBO is seasonally synchronous. Correspondence: Suvarna Fadnavis, Physical Meteorology and Aerology Division, Indian Institute of Tropical Meteorology, Dr. Homi Bhabha Road, Pashan, Pune 411008, India  相似文献   

16.
Agricultural systems models are essential tools to assess potential climate change (CC) impacts on crop production and help guide policy decisions. In this study, impacts of projected CC on dryland crop rotations of wheat-fallow (WF), wheat-corn-fallow (WCF), and wheat-corn-millet (WCM) in the U.S. Central Great Plains (Akron, Colorado) were simulated using the CERES V4.0 crop modules in RZWQM2. The CC scenarios for CO2, temperature and precipitation were based on a synthesis of Intergovernmental Panel on Climate Change (IPCC 2007) projections for Colorado. The CC for years 2025, 2050, 2075, and 2100 (CC projection years) were super-imposed on measured baseline climate data for 15–17 years collected during the long-term WF and WCF (1992–2008), and WCM (1994–2008) experiments at the location to provide inter-annual variability. For all the CC projection years, a decline in simulated wheat yield and an increase in actual transpiration were observed, but compared to the baseline these changes were not significant (p > 0.05) in all cases but one. However, corn and proso millet yields in all rotations and projection years declined significantly (p < 0.05), which resulted in decreased transpiration. Overall, the projected negative effects of rising temperatures on crop production dominated over any positive impacts of atmospheric CO2 increases in these dryland cropping systems. Simulated adaptation via changes in planting dates did not mitigate the yield losses of the crops significantly. However, the no-tillage maintained higher wheat yields than the conventional tillage in the WF rotation to year 2075. Possible effects of historical CO2 increases during the past century (from 300 to 380 ppm) on crop yields were also simulated using 96 years of measured climate data (1912–2008) at the location. On average the CO2 increase enhanced wheat yields by about 30%, and millet yields by about 17%, with no significant changes in corn yields.  相似文献   

17.
The samples of water-soluble inorganic ions (WSIs), including anions (F?, Cl?, SO42?, NO3?) and cations (NH4+, K+, Na+, Ca2+, Mg2+) in 8 size-segregated particle matter (PM), were collected using a sampler (with 8 nominal cut-sizes ranged from 0.43 to 9.0 μm) from October 2008 to September 2009 at five sites in both polluted and background regions of a coastal city, Xiamen. The results showed that particulate matters in the fine mode (PM2.1, Dp < 2.1 μm) comprised large part of mass concentrations of aerosols, which accounted for 45.56–51.27%, 40.04–60.81%, 42.02–60.81%, and 40.46–57.07% of the total particulate mass in spring, summer, autumn, and winter, respectively. The water-soluble ionic species in the fine mode at five sampling sites varied from 15.33 to 33.82 (spring), 14.03 to 28.06 (summer), 33.47 to 72.52 (autumn), and 48.39 to 69.75 μg m? 3 (winter), respectively, which accounted for 57.30 ± 6.51% of the PM2.1 mass concentrations. Secondary pollutants of NH4+, SO42? and NO3? were the dominant contributors of WSIs, which suggested that pollutants from anthropogenic activities, such as SO2, NOx were formed in aerosols by photochemical reactions. The size distributions of Na+, Cl?, SO42? and NO3? were bimodal, peaking at 0.43–0.65 μm and 3.3–5.8 μm. Although some ions, such as NH4+ presented bimodal distributions, the coarse mode was insignificant compared to the fine mode. Ca2+ and Mg2+ exhibited unimodal distributions at all sampling sites, peaking at 2.1–3.3 μm, while K+ having a bimodal distributions with a major peak at 0.43–0.65 μm and a minor one at 3.3–4.7 μm, were used in most of samples. Seasonal and spatial variations in the size-distribution profiles suggested that meteorological conditions (seasonal patterns) and sampling locations (geographical patterns) were the main factors determining the formation of secondary aerosols and characteristics of size distributions for WSIs.  相似文献   

18.
Summary Convective Available Potential Energy (CAPE) is the driving force for thunderstorm development. CAPE is closely controlled by wet bulb temperature. The lightning activity measured by a network of ten lightning flash counters widely distributed across continental Australia was studied as a function of wet bulb temperature. At each of the stations, the monthly total of lightning ground flashes, N, increased sharply with the increase of the monthly mean daily maximum wet bulb temperature, Tw, max. The dependence was strongest in the tropics and became less pronounced at temperate latitudes. In Darwin (latitude 12° S), the lightning ground flash activity increased by over three orders of magnitude over a 7 °C range of Tw, max. The corresponding increases for Coffs Harbour (latitude 30° S) and for Melbourne (latitude 38° S) were about one and a half orders of magnitude and about half an order of magnitude, respectively, each over a 10 °C range of Tw, max. Power law approximations were derived for each of the ten stations and showed that the logarithm of N was directly proportional to the power, P, of Tw, max. The value of P showed a sharp exponential decrease with increasing latitude away from the equator.  相似文献   

19.
Ambient respirable particles (PM10; aerodynamic diameter ≤10 μm) collected in a tropical urban environment (Delhi, India) during December 2008-November 2009 were characterized with respect to 16 US EPA priority polycyclic aromatic hydrocarbons (PAHs) and 8 major and trace metals (Fe, Mn, Cd, Cu, Ni, Pb, Zn and Cr). Concentrations of Σ16PAHs (annual mean: 74.7 ± 50.7 ng m−3, range 22.1–258.4 ng m−3) and most metallic species were at least an order of magnitude greater than values reported from similar locations worldwide. Seasonal variations in Σ16PAHs were significant (p < 0.001) with highest levels in winter while crustal and anthropogenic metals showed significant but mutually opposite seasonal dependence. Statistically significant associations were observed between chemical species and various meteorological parameters. The PAH profile was dominated by combustion-derived large-ring species (~85%) that were essentially local in origin. Principal component analysis–multiple linear regression (PCA-MLR) apportioned four sources: crustal dust (73%), vehicular emission (21%), coal combustion (4%) and industrial emission (2%) that was further validated by hierarchical cluster analysis (HCA). Temporal trend analysis showed that crustal sources were predominant in summer (p < 0.05) while the remaining sources were most active in winter. Summertime intrusions of Saharan dust were identified with the help of aerosol maps and air parcel backward trajectories. Inhalation cancer risk assessment showed that up to 3,907 excess cancer cases (357 for PAHs, 122 for Cd, 2040 for Cr (VI) and 1387 for Ni) are likely in Delhi considering lifetime inhalation exposure to these chemicals at their current concentrations.  相似文献   

20.
Summary ?Above orographically structured terrain considerable differences of the regional wind field may be identified during large-scale extreme wind events. So far, these regional differences could not be resolved by climate models. To determine the relationships between large-scale atmospheric conditions, the influence of orography, and the regional wind field, data measured in the upper Rhine valley within the framework of the REKLIP Regional Climate Project were analyzed and calculations were made using the KAMM mesoscale model. In the area of the upper Rhine valley, ratios of the wind velocity in the Rhine valley at 10 m above ground level, νval, and the large-scale flow velocity, νlar, are between νval/νlar ≈ 0.1 and νval/νlar ≈ 1. The νval/νlar ratio exhibits a strong dependence on thermal stratification, δ, and decreases from νval/νlar ≈ 1 at δ = 0 K m−1 to νval/νlar ≈ 0.2 at δ = 0.0075 K m−1. In areas, where the lateral mountainous border of the Rhine valley is interrupted, the νval/νlar ratio increases again with increasing stability or decreasing Froude number. This is obviously due to flow around the Black Forest under stable stratification. It is demonstrated by model calculations that a complex wind field develops in the Rhine valley at small Froude numbers (Fr < 1) irrespective of the direction of large-scale flow. The νval/νlar ratio is characterized by small values in the direct lee side (νval/νlar ≈ 0.2) and high values on the windward side of the lateral mountainous border of the Rhine valley (νval/νlar ≈ 0.8). Received October 22, 2001; revised June 18, 2002; accepted June 23, 2002  相似文献   

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