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1.
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   

2.
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   

3.
A study of the oxidation mechanism of N-methyl pyrrolidinone (C5H9NO, NMP) initiated by hydroxyl radicals was made at EUPHORE at atmospheric pressure (1000 ± 10) mbar of air and ambient temperature (T = 300 ± 5 K). The main products were N-methyl succinimide (NMS) (52 ± 4)% and N-formyl pyrrolidinone (FP) (23 ± 9)%. The relative rate technique was used to determine the rate constants of OH with NMP, NMS and FP, the measured values were (in units of cm3 molecule − 1 s− 1): kNMP = (2.2 ± 0.4) × 10− 11, kNMS = (1.4 ± 0.3) × 10− 12 and kFP = (6 ± 1) × 10− 12. The results are presented and discussed in terms of the atmospheric impact.  相似文献   

4.
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   

5.
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   

6.
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   

7.
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   

8.
Ambient concentrations of polycyclic aromatic hydrocarbons (PAHs) were measured in Helsinki (Finland). Particle mass size distributions were obtained with a cascade impactor (12 stages) with glass fibre filters as substrates. Simultaneously with the impactor measurements, particulate and gaseous PAHs were collected on a quartz filter and XAD-2 adsorbent, respectively, for evaluation of gas-partition coefficients. Samples were analysed for PAHs by on-line coupled supercritical fluid extraction — liquid chromatography — gas chromatography — mass spectrometry. The impactor results showed that most of the PAHs in Helsinki urban area were concentrated in fine particles (<2.5 μm diameter) with unimode peak at about 1 μm. The results were comparable with the number distribution measured with a differential mobility particle sizer. Total amounts of PAHs (gas + particle) varied from 15 (acenaphthylene) to 1990 (fluorene) pg/m3. The PAHs lighter than 202 amu (pyrene and fluoranthene) were exclusively in gas phase, whereas those heavier than 202 amu were mostly associated with particles. A plot of the partition coefficients (logKp) versus the temperature dependent sub-cooled vapour pressures (logp L 0 ) showed a gradient of −0.66, which deviated from equilibrium state (gradient = −1).  相似文献   

9.
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   

10.
In the present study, an attempt has been made to examine the governing photochemical processes of surface ozone (O3) formation in rural site. For this purpose, measurements of surface ozone and selected meteorological parameters have been made at Anantapur (14.62°N, 77.65°E, 331 m asl), a semi-arid zone in India from January 2002 to December 2003. The annual average diurnal variation of O3 shows maximum concentration 46 ppbv at noon and minimum 25 ppbv in the morning with 1σ standard deviation. The average seasonal variation of ozone mixing ratios are observed to be maximum (about 60 ppbv) during summer and minimum (about 22 ppbv) in the monsoon period. The monthly daytime and nighttime average surface ozone concentration shows a maximum (55 ± 7 ppbv; 37 ± 7.3 ppbv) in March and minimum (28 ± 3.4 ppbv; 22 ± 2.3 ppbv) in August during the study period. The monthly average high (low) O3 48.9 ± 7.7 ppbv (26.2 ± 3.5 ppbv) observed at noon in March (August) is due to the possible increase in precursor gas concentration by anthropogenic activity and the influence of meteorological parameters. The rate of increase of surface ozone is high (1.52 ppbv/h) in March and lower (0.40 ppbv/h) in July. The average rate of increase of O3 from midnight to midday is 1 ppbv/h. Surface temperature is highest (43–44°C) during March and April months leading to higher photochemical production. On the other hand, relative humidity, which is higher during the rainy season, shows negative correlation with temperature and ozone mixing ratio. It can be seen that among the two parameters are measured, correlation of surface ozone with wind speed is better (R 2=0.84) in compare with relative humidity (R 2=0.66).  相似文献   

11.
Using a database of spectra collected with an airborne infrared spectrometer between 1978 and 2005, the longest record of this type, we have searched for a temporal trend in the stratospheric OCS amount. The total column above 200 hPa, in latitudes from 30° to 60°N, shows a change of about 0.77 ± 0.80% per year relative to the 2010 value which is 1.34 × 1015 molecules cm−2; thus not a significant change. Observations are made from the base of the stratosphere and are uniquely suited to determining the stratospheric OCS abundance.  相似文献   

12.
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   

13.
This paper presents the main experimental results of surface ozone concentrations measured at a rural area in Northern Spain from February 2000 to December 2005. Daily and seasonal variation of ozone has been analysed. The peak concentration levels are obtained in the afternoon, mean value around 88 μg m−3, with extreme average values of 59 μg m−3 in January and 113 μg m−3 in July. Small differences are found in the mean and median of the ozone levels from April to August, when spring and summer maxima are observed. Despite the great inter-annual ozone variability obtained, most air quality indicators showed a positive trend. Further analysis of the monthly mean ozone concentrations of the main percentiles have also been performed using a harmonic model. The upward trend was 6.2 ± 1.7 μg m−3 for the 98th percentile. To interpret the main features of the annual cycle and describe the ozone peaks, the influence of meteorological factors is studied. In summer, ozone production is governed by local processes, air temperature being the major controlling factor. However, the origin of the spring maximum is not so well identified.  相似文献   

14.
Emissions of Polycyclic aromatic hydrocarbons by savanna fires   总被引：2，自引：0，他引：2  
Although Polycyclic aromatic hydrocarbons (PAH) are known as anthropogenic compounds arising from the combustion or the pyrolysis of fossil fuels, they may be also emitted by the combustion of vegetation. A field study was carried out in January 1991 at Lamto (Ivory Coast) as part of the FOS DECAFE experiment (Fire Of Savanna). Some ground samplings were devoted to the qualitative and quantitative characterization of atmospheric emissions by savanna fires during prescribed burns and under background conditions. Specific collections for gaseous and particulate PAHs have shown that the African practice of burning the savanna biomass during the winter months is an important source of PAHs. These compounds are emitted mainly in gaseous form but a significant fraction, essentially heavy PAHs, is associated with fine carbonaceous particles and can therefore represent a hazard for human health, since some of these compounds are mutagenic and carcinogenic. Twelve compounds were identified during the fire episodes and in the atmospheric background. The total concentration in the fires is of the order of 10 ng m–3 for the gas phase and from 0.1 to 1 ng m–3 in the aerosols. In the atmospheric background the mean concentrations are regular, 0.15 ng m–3 and 2 pg m–3, respectively. These concentrations are comparable with what is observed in European rural zones. The particulate emissions of PAHs by the savanna fires are distinguished by the abundance of some compounds which can be considered as tracers, although they are also slightly emitted by fossil fuel sources. These compounds are essentially pyrene, chrysene and coronene. In the gas phase, although no individual PAH may be considered as specific of the biomass combustion emissions, the relative abundances of the main PAHs are characteristic of the biomass burning. The concentrations of pyrene and fluorene are always predominant; these compounds could be considered as characteristic emission products of smoldering and flaming episodes, respectively. In the background the PAH composition shows that in a tropical region the air consists of a mixture coming from the various sources, but the biomass combustion is by far the most important source.The fluxes of total PAH emitted by savanna biomass burning in Africa were estimated to be of the order of 17 and 600 ton yr–1, respectively, for the particulate PAHs and the gaseous PAHs, respectively.  相似文献   

15.
Ozone tendencies due to chemistry and transport are calculated by a mesoscale model using a fine horizontal resolution (3 km × 3 km), over South-Eastern France. Over that region where the anthropogenic emissions are very strong, ozone pollution is highlighted during two intensive observations periods of the ESCOMPTE campaign, when the sea breeze penetrates far into the Durance and Rhone valleys and the up-slope breezes are developed. From a fine analysis of time series of ozone concentration at different ground stations along these valleys and from numerical results, it is possible to discriminate the tendency due to chemistry from the tendency due to dynamical processes. We can distinguish both processes, either local chemical production/loss or dynamical increase/decrease (transport, deposition) on maps of ozone budget according to the meteorological conditions. In particular, we show that the variations due to transport can be have the same order of magnitude than those due to chemistry, reaching 20 ppbv h−1, whereas those due to chemistry are around 30 ppbv h−1.  相似文献   

16.
Simulations of polar ozone losses were performed using the three-dimensional high-resolution (1∘ × 1∘) chemical transport model MIMOSA-CHIM. Three Arctic winters 1999–2000, 2001–2002, 2002–2003 and three Antarctic winters 2001, 2002, and 2003 were considered for the study. The cumulative ozone loss in the Arctic winter 2002–2003 reached around 35% at 475 K inside the vortex, as compared to more than 60% in 1999–2000. During 1999–2000, denitrification induces a maximum of about 23% extra ozone loss at 475 K as compared to 17% in 2002–2003. Unlike these two colder Arctic winters, the 2001–2002 Arctic was warmer and did not experience much ozone loss. Sensitivity tests showed that the chosen resolution of 1∘ × 1∘ provides a better evaluation of ozone loss at the edge of the polar vortex in high solar zenith angle conditions. The simulation results for ozone, ClO, HNO3, N2O, and NO y for winters 1999–2000 and 2002–2003 were compared with measurements on board ER-2 and Geophysica aircraft respectively. Sensitivity tests showed that increasing heating rates calculated by the model by 50% and doubling the PSC (Polar Stratospheric Clouds) particle density (from 5 × 10−3 to 10−2 cm−3) refines the agreement with in situ ozone, N2O and NO y levels. In this configuration, simulated ClO levels are increased and are in better agreement with observations in January but are overestimated by about 20% in March. The use of the Burkholder et al. (1990) Cl2O2 absorption cross-sections slightly increases further ClO levels especially in high solar zenith angle conditions. Comparisons of the modelled ozone values with ozonesonde measurement in the Antarctic winter 2003 and with Polar Ozone and Aerosol Measurement III (POAM III) measurements in the Antarctic winters 2001 and 2002, shows that the simulations underestimate the ozone loss rate at the end of the ozone destruction period. A slightly better agreement is obtained with the use of Burkholder et al. (1990) Cl2O2 absorption cross-sections.  相似文献   

17.
Summary  Measurements of landscape-scale methane emission were made over an aapa mire near Kaamanen in Finnish Lapland (69° 8′ N, 27° 16′ E, 155 m ASL). Emissions were measured during the spring thaw, in summer and in autumn. No effect of water table position on CH4 emission was found as the water table remained at or above the surface of the peat. Methane emission fluxes increased with surface temperature from which an activation energy of −99 kJ mol−1 was obtained. Annual emission from the site, modelled from temperature regression and short-term flux measurements made in three separate years, was calculated to be 5.5 ± 0.4 g CH4 m−2 y−1 of which 0.6 ± 0.1 g CH4 m−2 y−1 (11%) was released during the spring thaw which lasted 20 to 30 days. The effect of global warming on the CH4 budget of the site was estimated using the central scenario of the SILMU (Finnish Research Programme on Climate Change) model which predicts annual mean temperature increases of 1.2, 2.4 and 4.4 °C in 2020, 2050 and 2100, respectively. Maximum enhancements in CH4 emission due to warming were calculated to be 18, 40 and 84% for 2020, 2050 and 2100, respectively. Actual increases may be smaller because prediction of changes in water table are highly uncertain. Received September 17, 1999 Revised October 16, 2000  相似文献   

18.
This article presents a complete study of the diurnal chemical reactivity of the biogenic volatile organic compound (BVOC), 2-methyl-3-buten-2-ol (MBO) in the troposphere. Reactions of MBO with OH and with ozone were studied to analyse the respective parts of both processes in the global budget of MBO atmospheric reactivity. They were investigated under controlled conditions for pressure (atmospheric pressure) and temperature (298 ± 2 K) using three complementary European simulation chambers. Reaction with OH radicals was studied in the presence of and in the absence of NO x . The kinetic study was carried out by relative rate study using isoprene as a reference. The rate constant found for this reaction was molecule−1 cm3 s−1. FTIR spectroscopy, DNPH- and PFBHA-derivatisation analyses were performed for reactions with both OH radicals and ozone. In both reactions, the hydroxycarbonyl compound, 2-hydroxy-2-methylpropanal (HMPr) was positively identified and quantified, with a yield of in the reaction with OH, and a yield of and 0.84 ± 0.08 in the reaction with ozone under dry (HR < 1%) and humid conditions (HR = 20%–30%). A primary production of two other carbonyl compounds, acetone , and formaldehyde was found in the case of the dry ozonolysis experiments. Under humid conditions, only formaldehyde was co-produced with HMPr as a primary carbonyl compound, with a yield of . For the reaction with OH, three other carbonyl compounds were detected, acetone , formaldehyde and glycolaldehyde . In addition some realistic photo-oxidation experiments were performed to understand in an overall way the transformations of MBO in the atmosphere. The realistic photo-oxidation experiments were conducted in the EUPHORE outdoor simulation chamber. It was found that this compound is a weak secondary aerosol producer (less than 1% of the carbon balance). But it was confirmed that it is a potentially significant source of acetone, Δ[Acetone]/Δ[MBO] = 0.45. With our experimental conditions ([MBO]0 = 200 ppb, [NO]o = 50 ppb), an ozone yield of Δ[O3]/Δ[MBO] = 1.05 was found.  相似文献   

19.
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   

20.
The concentrations of PM10, PM2.5 and their water-soluble ionic species were determined for the samples collected during January to December, 2007 at New Delhi (28.63° N, 77.18° E), India. The annual mean PM10 and PM2.5 concentrations (± standard deviation) were about 219 (± 84) and 97 (±56) μgm−3 respectively, about twice the prescribed Indian National Ambient Air Quality Standards values. The monthly average ratio of PM2.5/PM10 varied between 0.18 (June) and 0.86 (February) with an annual mean of ∼0.48 (±0.2), suggesting the dominance of coarser in summer and fine size particles in winter. The difference between the concentrations of PM10 and PM2.5, is deemed as the contribution of the coarse fraction (PM10−2.5). The analyzed coarse fractions mainly composed of secondary inorganic aerosols species (16.0 μgm−3, 13.07%), mineral matter (12.32 μgm−3, 10.06%) and salt particles (4.92 μgm−3, 4.02%). PM2.5 are mainly made up of undetermined fractions (39.46 μgm−3, 40.9%), secondary inorganic aerosols (26.15 μgm−3, 27.1%), salt aerosols (22.48 μgm−3, 23.3%) and mineral matter (8.41 μgm−3, 8.7%). The black carbon aerosols concentrations measured at a nearby (∼300 m) location to aerosol sampling site, registered an annual mean of ∼14 (±12) μgm−3, which is significantly large compared to those observed at other locations in India. The source identifications are made for the ionic species in PM10 and PM2.5. The results are discussed by way of correlations and factor analyses. The significant correlations of Cl−, SO42−, K+, Na+, Ca2+, NO3− and Mg2+ with PM2.5 on one hand and Mg2+ with PM10 on the other suggest the dominance of anthropogenic and soil origin aerosols in Delhi.  相似文献   

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