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1.
PM10 samples were collected over three years at Monzenmachi, the Japan Sea coast, the Noto Peninsula, Ishikawa, Japan from January 17, 2001 to December 18, 2003, using a high volume air sampler with quartz filters. The concentrations of the water-soluble inorganic ions in PM10 were determined with using ion chromatography. By analyzing the characteristics of these, the evidences were found that the Asian outflow had an obviously influence on the air quality at our study site. The results were as follows: the secondary pollutants SO42−, NO3− and NH4+ were the primary water-soluble inorganic ions at our study site. The monthly mean concentrations of SO42−, NH4+, NO3− and Ca2+ have prominent peak in spring due to the strong influence of the Asian continent outflow—these according to backward air trajectory analysis, the maximum of which were 6.09 for nss-SO42− in May, 2.87 for NO3− and 0.68 μg m−3 for nss-Ca2+ in April, respectively. Comparable to similar data reported from various points around East Asia, it had the characteristics of a polluted coastal area at our study site. The concentration of nss-Ca2+ in PM10 drastically increased when the Asian dust invaded, the mean value during the Asian dust days(AD) was 0.86 μg m−3, about 4 times higher than those of normal days (NAD). Meanwhile, the mean concentrations of nss-SO42−, NO3− and NH4+ in AD periods were higher than those in NAD periods which were 5.87, 1.76 and 1.82 μg m−3, respectively, it is due to the interaction between dust and secondary particles during the long-range transport of dust storms. Finally, according to the source apportionment with positive matrix factorization (PMF) method in this study, the major source profiles of PM10 at our study site were categorized as (1) marine salt, (2) secondary sulfate, (3) secondary nitrate and (4) crustal source.  相似文献   

2.
Samples of rain water were collected during monsoon season (June to September) of 2006 and 2007 at Hudegadde, a rural site located in an ecological sensitive area of Western Ghats. The collected samples were analyzed for pH, conductivity and major ions. At this site, rainwater pH varied from 4.20 to 7.39 with 5.65 as volume weighed mean. The observed mean was slightly lower than the average pH reported at most of the Indian continental sites. Monthly variation showed that average pH of rain water was the lowest during September (end of monsoon) and the highest during July (peak of monsoon). Overall, marine sources had dominating influence at this site. However, significant influence of anthropogenic and crustal sources from local as well as inter-continental regions was also noticed. As compared to NO3−, higher concentration of SO42− was noticed which might be due to contribution from industrial activities responsible for SO2 emission. At this site, influence of five types of airmass trajectories was noticed i.e. i) C.I.O. (Central part of Indian Ocean)-when air masses blown from Maldives and nearby region of central Indian ocean. These airmasses had higher concentrations of nss Ca2+ which did not show any adverse impact on the pH; ii) N.W.I.O.(North-West Indian Ocean)-when airmasses travelled from oceanic region close to north-east Africa. These airmassses had higher concentrations of nss sulphate and nitrate and gave rise to acid rain; iii) S.W.I.O. (South -West Indian Ocean)- when airmasses came from southern part of Indian ocean (close to Mauritius). During these airmasses, rain water samples had almost equal ratio of nss SO42− and nss Ca2+ similar to N.W.I.O but very low NO3− ; iv) Gulf-when airmasses were observed coming from Gulf region. Although these airmasses contributed only 2% of the total number of samples but carried high amount of nss SO42− which gave rise to acid rain. The second lowest pH was observed during these airmasses which might be due to very high nssSO42−/nssCa2+ ratios; v) N.W.I.O. + S.W.I.C. (North-West Indian Ocean+South-West Indian Continental)- when airmasses originated from north-west Indian Ocean travelling towards south continental part of India and then arriving to the site. During these airmasses, samples showed typical influence of urban activities having high concentrations of nss SO42− and NO3− leading to the lowest pH of rain water.  相似文献   

3.
Continuous weekly monitoring on the concentration of gases and aerosols in urban ambient air by a four-stage filter-pack method was carried out for 7 years in order to study not only the acid-base balance of acid-related (HNO3, NO3 −, and non-sea-salt-(nss-)SO4 2−) and alkali-related (NH3, NH4 +, and nss-Ca2+) chemical species but also its influence on the acidification of precipitation. The concentrations of the total nitrate (= NO3− + HNO3) and nss-SO42− showed a similar seasonal variation: high in the summer and low in the winter. The total nitrate and nss-SO42− accounted for 0.43 and 0.57 of the acid-related species, respectively, on an equivalent basis. The total ammonium (= NH3 + NH4+) accounted for more than 0.9 of the alkali-related species, except for a springtime nss-Ca2+ episodic peak. The alkali-related species were generally overabundant compared with the acid-related species in the HNO3-NO3−-nss-SO42−-NH3-NH4+-nss-Ca2+ system. The alkali-rich distribution was especially pronounced in the winter, but the acid-related species was comparable to the alkali-related species in the summer, which was attributed to the larger H+ deposition by precipitation in the summer. This study can provide a methodology to associate survey results obtained by a filter-pack method with those of precipitation.  相似文献   

4.
Measurements of fog and rain water chemistry at the summit of Mt. Fuji, the highest peak in Japan, as well as at Tarobo, the ESE slope of Mt. Fuji in September 2002. The pH of fog and rain water sampled at Mt. Fuji varied over a range of 4.0–6.8. Acidic fogs (pH < 5.0) were observed at the summit when the air mass came from the industrial regions on the Asian continent. The ratio of [SO42−]/[NO3−] in the fog water was lower at Tarobo than at the summit. High concentrations of Na+ and Cl− were determined in the rain water sampled at the summit, possibly because of the long-range transport of sea-salt particles raised by a typhoon through the middle troposphere. The vertical transport of sea-salt particles would influence the cloud microphysical properties in the middle troposphere. Significant loss of Mg2+ was seen in the rain water at the summit. The concentrations of peroxides in the fog and rain water were relatively large (10–105 μM). The potential capacity for SO2 oxidation seems to be strong from summer to early autumn at Mt. Fuji. The fog water peroxide concentrations displayed diurnal variability. The peroxide concentrations in the nighttime were significantly higher than those in the daytime.  相似文献   

5.
Cloud/fog samples were collected during spring of 2007 in the highly polluted North China Plain in order to examine the impact of pollution and dust particles on cloud water chemistry. The volume weighted mean pH of cloud water was 3.68. The cloud acidity was shown to be associated with air mass origins. Cloud water with its air mass trajectories originating from the southern part of China was more acidic than those from northern China. Anthropogenic source and dust had obvious impact on cloud water composition as indicated by the very high mean concentrations of SO42? (1331.65 μeq L? 1), NO3? (772.44 μeq L? 1), NH4+ (1375.92 μeq L? 1) and Ca2+ (625.81 μeq L? 1) in the observation periods. During sandstorm days, cloud pH values were relatively high, and the concentrations of all the ions in cloud water reached unusual high levels. Significant decreases in the mass concentrations of PM2.5 and PM10 were observed during cloud events. The average scavenging ratio for PM2.5 and PM10 was 52.0% and 55.7%, respectively. Among the soluble ions in fine particles, NO3?, K+ and NH4+ tend to be more easily scavenged than Ca2+ and Na+.  相似文献   

6.
The new European Council Directive (PE-CONS 3696/07) frames the inhalable (PM10) and fine particles (PM2.5) on priority to chemically characterize these fractions in order to understand their possible relation with health effects. Considering this, PM2.5 was collected during four different seasons to evaluate the relative abundance of bulk elements (Cl, S, Si, Al, Br, Cu, Fe, Ti, Ca, K, Pb, Zn, Ni, Mn, Cr and V) and water soluble ions (F−, Cl−, NO2 −, NO3 −, SO4 2−, Na+, NH4 +, Ca2+ and Mg2+) over Menen, a Belgian city near the French border. The air quality over Menen is influenced by industrialized regions on both sides of the border. The most abundant ionic species were NO3 −, SO4 2− and NH4 +, and they showed distinct seasonal variation. The elevated levels of NO3 − during spring and summer were found to be related to the larger availability of the NOx precursor. The various elemental species analyzed were distinguished into crustal and anthropogenic source categories. The dominating elements were S and Cl in the PM2.5 particles. The anthropogenic fraction (e.g. Zn, Pb, and Cu) shows a more scattered abundance. Furthermore, the ions and elemental data were also processed using principal component analysis and cluster analysis to identify their sources and chemistry. These approach identifies anthropogenic (traffic and industrial) emissions as a major source for fine particles. The variations in the natural/anthropogenic fractions of PM2.5 were also found to be a function of meteorological conditions as well as of long-range transport of air masses from the industrialized regions of the continent. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.  相似文献   

7.
Long-term measurements of ambient particulate matter less than 2.5 μm in diameter (PM2.5) and its chemical compositions were performed at a rural site in Korea from December 2005 to August 2009. The average PM2.5 concentration was 31 μg m−3 for the whole sampling period, and showed a slightly downward annual trend. The major components of PM2.5 were organic carbon, SO42−, NO3−, and NH4+, which accounted for 55 % of total PM2.5 mass on average. For the top 10 % of PM2.5 samples, anionic constituents and trace elements clearly increased while carbonaceous constituents and NH4+ remained relatively constant. Both Asian dust and fog events clearly increased PM2.5 concentrations, but affected its chemical composition differently. While trace elements significantly increased during Asian dust events, NO3−, NH4+ and Cl were dramatically enhanced during fog events due to the formation of saturated or supersaturated salt solution. The back-trajectory based model, PSCF (Potential Source Contribution Function) identified the major industrial areas in Eastern China as the possible source areas for the high PM2.5 concentrations at the sampling site. Using factor analysis, soil, combustion processes, non-metal manufacture, and secondary PM2.5 sources accounted for 77 % of the total explained variance.  相似文献   

8.
In this paper, the basic composition of fog and low cloud water are presented, resulting from the analyses of water samples from 111 fog/cloud events. The samples were collected at five sites located in various regions of the Czech Republic. Two sampling sites are in mountainous regions and three sites represent various urban areas. The mountain stations are located in two regions of the Czech Republic with different industry types. At all the sites, active fog collectors were employed. In the water samples, the conductivity, acidity (pH), cations (H+, Na+, K+, NH4+, Mg2+, Ca2+) and anions (F−, Cl−, NO3−, SO42−) were determined.A mean pH value of about 4.5 was obtained at mountain sites whereas the measurements in urban areas showed mean pH values from 4.9 to 6.4. The mean conductivity values in the samples from the two mountain stations were 137 and 191.5 μS cm−1. The samples from urban sites showed mean values between 127.7 and 654.4 μS cm−1. The maximum concentration means for the three dominant pollutants (expressed by the ratio mountain sites/urban sites) are 32.9/99.6 mg l−1 for NO3−, 32.5/192.9 mg l−1 for SO42− and 18.5/52.7 mg l−1 for NH4+. As expected, we found higher ion concentrations in the northern part of the Czech Republic where larger numbers of lignite-burning power plants, chemical factories and opencast lignite mines are located. A decrease in ion concentrations was observed at higher altitude sites, probably reflecting at least in part higher liquid water contents at these locations.  相似文献   

9.
Secondary aerosol formation was studied at Allahabad in the Indo-Gangetic region during a field campaign called Land Campaign-II in December 2004 (northern winter). Regional source locations of the ionic species in PM10 were identified by using Potential Source Contribution Function (PSCF analysis). On an average, the concentration of water soluble inorganic ions (sum of anions and cations) was 63.2 μgm−3. Amongst the water soluble ions, average NO3− concentration was the highest (25.0 μgm−3) followed by SO42− (15.8 μgm−3) and NH4+ (13.8 μgm−3) concentrations. These species, contributed 87% of the total mass of water soluble species, indicating that most of the water soluble PM10 was composed of NH4NO3 and (NH4)2SO4/NH4HSO4 or (NH4)3H(SO4)2 particles. Further, the concentrations of SO42−, NO3−, and NH4+ aerosols increased at high relative humidity levels up to the deliquescence point (∼63% RH) for salts of these species suggesting that high humidity levels favor the conversion and partitioning of gaseous SO2, NOx, and NH3 to their aerosol phase. Additionally, lowering of ambient temperature as the winter progressed also resulted in an increase of NO3− and NH4+ concentrations, probably due to the semi volatile nature of ammonium nitrate. PSCF analysis identified regions along the Indo-Gangetic Plain (IGP) including Northern and Central Uttar Pradesh, Punjab, Haryana, Northern Pakistan, and parts of Rajasthan as source regions of airborne nitrate. Similar source regions, along with Northeastern Madhya Pradesh were identified for sulfate.  相似文献   

10.
A suite of active and passive remote sensing instruments and in-situ sensors deployed at the SIRTA Observatory (Instrumented Site for Atmospheric Remote Sensing Research), near Paris, France, for a period of six months (October 2006–March 2007) document simultaneously radiative, microphysical and dynamic processes driving the continental-fog life cycle. The study focuses on a 6-day period between 23 and 29 December 2006 characterized by several stratus-cloud lowering and lifting events and almost 18 h of visibility below 1 km. Conceptual models and different possible scenarios are presented here to explain the formation, the development and the dissipation phases of three major stratus–fog events and to quantify the impact of each driving process. For example, slowly evolving large-scale conditions characterized by a slow continuous cloud-base lowering, followed by a rapid transient period conductive to fog formation and dissipation, are observed for cases 1 and 3. During this stable period, continuous cloud-top radiative cooling (≈ −160 Wm−2) induces a progressive and slow lowering of the cloud base: larger droplets at cloud top (cloud reflectivity approximately equals to −20 dBZ) induce slow droplet fall to and beyond cloud base (Doppler velocity ≈ −0.1 ms−1), cooling the sub-cloud layer by evaporation and lowering the saturation level to 100 m (case 1) or to the surface (cases 2 and 3). Suddenly, a significant increase in Doppler velocity magnitude ≈ −0.6 ms−1 and of turbulent kinetic energy dissipation rate around 10−3 m2s−3 occurs at cloud base (case 1). These larger cloud droplets reach the surface leading to fog formation over 1.5 h. The Doppler velocity continues to increase over the entire cloud depth with a maximum value of around −1 ms−1 due to the collection of fog droplets by the drizzle drops with high collection efficiency. As particles become larger, they fall to the ground and lead to fog dissipation. Hence, falling particles play a major role in both the formation and also in the dissipation of the fog. These roles co-exist and the balance is driven by the characteristics of the falling particles, such as the concentration of drizzle drops, the size distribution of drizzle drops compared to fog droplets, Doppler velocity and thermodynamic state close to the surface.  相似文献   

11.
A comprehensive study on the chemical compositions of rainwater was carried out from June 2007 to December 2008 in Guiyang, a city located on the acid rain control zone of southwest China. All samples were analyzed for pH, major anions (F−, Cl−, NO3−, SO42−), major cations (K+, Na+, Ca2+, Mg2+, NH4+), Sr2+ and Sr isotope. The pH increase is due to the result of neutralization caused by the alkaline dust which contain large amount of CaCO3. It was observed that Ca2+ was the most abundant cation with a volume-weighted mean (VWM) value of 217.6 μeq/L (52.7–1928 μeq/L), accounting for 66% (39%–88%) of the total cations. SO42− was the most abundant anion with VWM value of 237.8 μeq/L (49.6-1643 μeq/L). SO42− and NO3− were dominant among the anions, accounting for 66%–97% of the total measured anions. The Sr concentrations vary from 0.01 to 0.92 μmol/L, and strontium isotopic ratios vary in the range of 0.707684–0.710094, with an average of 0.708092. The elements ratios and the 87Sr/86Sr ratios showed that the solutes of rainwater mainly come from weathering of carbonate and secondary dust input. Moreover, urbanization results in the calcium-rich dust increased and the high concentrations of alkaline ions (mainly Ca2+) have played an important role to neutralize the acidity of rainwater, leading to the increase of arithmetic pH mean value by 0.5 units since 2002. It is worth noting that the emission of SO2 and NOx from the automobile exhaust is increasing and is becoming another important precursor of acid rain now.  相似文献   

12.
Measurements of atmospheric dimethylsulfide (DMS) and its oxidation products, sulfur dioxide (SO2), methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2-) were monitored during the period June 9–26, 1989 at a coastal site in Brittany. As indicated by the radon (Rn-222) activities and the high concentrations of NOx the air masses, for most of the experiment, were continental in origin. The observed concentrations range from 1.9 to 65 nmol/m3 for DMS (n=157), 0.6 to 94.2 nmol/m3 for SO2 (n=50), 0.6 to 11.6 nmol/m3 for MSA (n=44) and 42 to 350 nmol/m3 for nss-SO4 2- (n=44). Aitken nuclei reached values as high as 4.5 × 105 particles/m3. When continental conditions predominated, the measured SO2 concentrations were lower than those expected from a consideration of the observed DMS concentrations and the existence of SO2 background of the continental air masses. Similarly, compared to the MSA/DMS ratio in the marine atmosphere, higher concentrations of MSA were observed than those expected from the measured levels of DMS. The presence of enhanced levels of MSA was also endorsed by the observation that the measured mean MSA/nss-SO4 2- ratio of 6±3% was similar to the mean value of 6.9% observed in the marine atmosphere. These above observations are in line with recent laboratory findings by Barnes et al. (1988), which show an increase of the MSA/DMS yield with a simultaneous decrease of the SO2/DMS yield in the presence of NOx.  相似文献   

13.
The chemistry of heavy haze over Urumqi,Central Asia   总被引：1，自引：0，他引：1  
A sampling campaign of aerosols over Urumqi from 2001–2007 and soil samples in the surrounding areas were carried out to investigate the severe air pollution in Urumqi, a typical inland city, located in the center of Asia. Urumqi is one of the heavy polluted cities in the world, as the days of haze spanned over one third of the year and accounted for 60–80% of the heating period for the past 6 years. High concentration of fine aerosols, frequent occurrence, and rapid formation of heavy haze were the three main characteristics. With comparison of the pollution elements, As, Cd, and S, and the ratio of Ca/Al in aerosols and soils in those sites located on the south of Jungger Basin as tracers, it was found that As, Cd, and S highly enriched in the aerosols over urban Urumqi were not only from the re-suspended road dust but also from the soil transported from south of the Jungger Basin. Different from the most cities in China, the high concentration of sulfate in Urumqi was partially from the primary soil dust transported from the surrounding areas. The mixing of the local anthropogenic aerosols with the soil transported from outside the city was the main source of the high sulfate concentration. Ammonium salts were higher than the summed equivalents of SO42−, NO3−, and Cl− in Urumqi and much higher than that in other Chinese cities. The total water soluble ions and the total ammonium salts were as high as 57.8% and 51.0% in PM2.5. The high concentration of soluble salts with high hygroscopicity, especially ammonium and sulfate salts, were the main factors contributing to the heavy haze over Urumqi.  相似文献   

14.
The dynamics and the aerosol chemistry of the air masses reaching the free troposphere of the subtropical Northeast Atlantic region during the period 1995–98 have been studied. Seven days backward trajectories were calculated daily with HYSPLIT-4 model for Izaña Global Atmospheric Watch (GAW) Observatory (28.3°N 16.5°W, 2367 m a.s.l.). These back-trajectories were classified by means of a k-means clustering strategy. The daily air masses have been coded using 16 variables to detect the aerosol load of each one of them. Four clusters were found: Cluster 1, representative of Atlantic oceanic middle troposphere air masses, (OMT), has an average frequency of occurrence of 50.6%. Cluster 2, which includes air masses originated in the African continent (AfD), has been recorded in a 19.8% of time. Cluster 3 represents a mixture at least of two of the next sources: Europe, Africa and Ocean, (EAM), with a frequency of 12.7%. Finally, Cluster 4 includes air masses with a high load of maritime aerosols, (MaA), and it has been detected in a 16.9%. An analysis of four aerosol components: NO3 ?, NH4 +, non-sea-salt-SO4 2?, and mineral dust and its relation with the origin and transport of the air masses have been done. The highest quantities of mineral dust and nss-SO4 2? are linked with African air masses with a mean value of 86.5 and 1.9 μg/m3 respectively. Whereas the highest levels of NO3 ?, 1.0 μg/m3, and NH4 +, 0.4 μg/m3, were obtained for AfD and EAM. The lowest levels were associated with OMT and MaA air masses types: 12.7, 0.6, 0.2, and 0.5 μg/m3 for dust, NO3 ?, NH4 +, and nss-SO4 2? in average for the four studied years. However, it is remarkable that the values of the median for dust are 2.2 and 3.5 μg/m3 in clusters MaA and OMT respectively. Using non-parametric statistical tests the distributions of concentrations in each cluster by year have been compared in order to detect similarities. The results show that the aerosol loads of OMT and MaA air masses are quite similar and the same occurs for AfD and EAM air masses. However, the correlation analysis between the levels of anions and ammonium evidenced important differences among the air mass types. In AfD air masses is clear a low correlation between levels of nss-SO4 2? and NH4 + (r 2 = 0.08) suggesting that the sulfate speciation was dominated by sulfate species others than ammonium sulfate, such as calcium sulfate. CaSO4 ?2H2O (gypsum) is mainly present in the coarse mode, where the radiative effects of sulfate are less important that in the accumulative mode. For OMT air masses is noticeable an important increasing on the correlation between the levels of anions and those of NH4 + for the two last years of the study period (1997–1998, r 2 = 0.61 –0.85%) with respect to the first ones (1995–1996, r 2 = 0.25–0.49%), coinciding with the second strongest ENSO (El Niño Southern Oscillation) event recorded. This behavior indicates a change in the speciation of the aerosol component.  相似文献   

15.
Dimethylsulfide (DMS), sulfur dioxide (SO2), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO4 2–), sodium (Na+), ammonium (NH4 +), and nitrate (NO3 –) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m–3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m–3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.The atmospheric SO2 concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m–3 (STP). The nonsea-salt sulfate (ns-SO4 2–) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO2 and nss-SO4 2– from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a sea-salt inversion layer was reflected in the profiles of those aerosol components, e.g., Na+ and NO3 –, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently remote northern hemispheric regions.  相似文献   

16.
Simultaneous measurements on physical, chemical and optical properties of aerosols over a tropical semi-arid location, Agra in north India, were undertaken during December 2004. The average concentration of total suspended particulates (TSP) increased by about 1.4 times during intense foggy/hazy days. Concentrations of SO4 2−, NO3 −, NH4 + and Black Carbon (BC) aerosols increased by 4, 2, 3.5 and 1.7 times, respectively during that period. Aerosols were acidic during intense foggy/hazy days but the fog water showed alkaline nature, mainly due to the neutralizing capacity of NH4 aerosols. Trajectory analyses showed that air masses were predominantly from NW direction, which might be responsible for transport of BC from distant and surrounding local sources. Diurnal variation of BC on all days showed a morning and an evening peak that were related to domestic cooking and vehicular emissions, apart from boundary layer changes. OPAC (Optical properties of aerosols and clouds) model was used to compute the optical properties of aerosols. Both OPAC-derived and observed aerosol optical depth (AOD) values showed spectral variation with high loadings in the short wavelengths (<1 μm). AOD value at 0.5 μm wavelength was significantly high during intense foggy/hazy days (1.22) than during clear sky or less foggy/hazy days (0.63). OPAC-derived Single scattering albedo (SSA) was 0.84 during the observational period, indicating significant contribution of absorbing aerosols. However, the BC mass fraction to TSP increased by only 1% during intense foggy/hazy days and thereby did not show any impact on SSA during that period. A large increase was observed in the shortwave (SW) atmospheric (ATM) forcing during intense foggy/hazy days (+75.8 W/m2) than that during clear sky or less foggy/hazy days (+38 W/m2), mainly due to increase in absorbing aerosols. Whereas SW forcing at surface (SUF) increased from −40 W/m2 during clear sky or less foggy/hazy days to −76 W/m2 during intense foggy/hazy days, mainly due to the scattering aerosols like SO4 2-.  相似文献   

17.
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   

18.
Vertical distributions of dimethylsulfide (DMS), sulfur dioxide (SO2), aerosol methane-sulfonate (MSA), non-sea-salt sulfate (nss-SO4 2-), and other aerosol ions were measured in maritime air west of Tasmania (Australia) during December 1986. A few cloudwater and rainwater samples were also collected and analyzed for major anions and cations. DMS concentrations in the mixed layer (ML) were typically between 15–60 ppt (parts per trillion, 10–12; 24 ppt=1 nmol m–3 (20°C, 1013 hPa)) and decreased in the free troposphere (FT) to about <1–2.4 ppt at 3 km. One profile study showed elevated DMS concentrations at cloud level consistent with turbulent transport (cloud pumping) of air below convective cloud cells. In another case, a diel variation of DMS was observed in the ML. Our data suggest that meteorological rather than photochemical processes were responsible for this behavior. Based on model calculations we estimate a DMS lifetime in the ML of 0.9 days and a DMS sea-to-air flux of 2–3 mol m–2 d–1. These estimates pertain to early austral summer conditions and southern mid-ocean latitudes. Typical MSA concentrations were 11 ppt in the ML and 4.7–6.8 ppt in the FT. Sulfur-dioxide values were almost constant in the ML and the lower FT within a range of 4–22 ppt between individual flight days. A strong increase of the SO2 concentration in the middle FT (5.3 km) was observed. We estimate the residence time of SO2 in the ML to be about 1 day. Aqueous-phase oxidation in clouds is probably the major removal process for SO2. The corresponding removal rate is estimated to be a factor of 3 larger than the rate of homogeneous oxidation of SO2 by OH. Model calculations suggest that roughly two-thirds of DMS in the ML are converted to SO2 and one-third to MSA. On the other hand, MSA/nss-SO4 2- mole ratios were significantly higher compared to values previously reported for other ocean areas suggesting a relatively higher production of MSA from DMS oxidation over the Southern Ocean. Nss-SO4 2- profiles were mostly parallel to those of MSA, except when air was advected partially from continental areas (Africa, Australia). In contrast to SO2, nss-SO4 2- values decreased significantly in the middle FT. NH4 +/nss-SO4 2- mole ratios indicate that most non-sea-salt sulfate particles in the ML were neutralized by ammonium.  相似文献   

19.
The chemistry of cloud multiphase systems was studied within the Kleiner Feldberg Cloud Experiment 1990. The clouds encountered during this experimental campaign could be divided into two categories according to the origin of air masses in which the clouds formed. From the chemical point of view, clouds passing the sampling site during the first period of the campaign (26 October-4 November) were characterized by lower pollutant loading and higher pH, as compared to clouds during the final period of the experimental campaign (10–13 November). The study of multiphase partitioning of the main chemical constituents of the cloud systems and of atmospheric acidity within the multiphase systems themselves (gas + interstitial aerosol + liquid droplets) are presented in this paper. A general lack of gaseous NH3 was found in these cloud systems, which caused a lack of buffer capacity toward acid addition. Evidence supports the hypothesis that the higher acidity of the cloud systems during this final period of the campaign was due to input of HNO3. Our measurements, however, could not determine whether the observed input was due to scavenging of gaseous HNO3 from the air feeding into the cloud, or to heterogeneous HNO3 formation via NO2 oxidation by O3 to NO3 and N2O5. Sulfate in cloud droplets mainly originated from aerosol SO 4 2– scavenging, since S(IV) to S(VI) liquid phase conversion was inhibited due to both lack of H2O2 and low pH of cloud droplets, which made O3 and metal catalyzed S(IV) oxidation inefficient.  相似文献   

20.
Using a single drop experiment, the uptake of NO3 radicals on aqueous solutions of the dye Alizarin Red S and NaCl was measured at 293 K. Uptake coefficients in the range (1.7–3.1) ⋅ 10− 3 were measured on Alizarin Red S solutions. The uptake coefficients measured on NaCl solutions were in the range of (1.1–2.0) ⋅ 10−3 depending on the salt concentration. Both experiments lead to a consistent result for the mass accommodation coefficient of αNO3 = (4.2− 1.7+2.2)⋅ 10−3. The product H(Dl kCl−II)0.5 for the NO3 radical was determined to be (1.9 ± 0.2) M atm− 1 cm s−0.5 M−0.5 s−0.5 by fitting the uptake data for the NaCl solutions to the so-called resistance model. The yield of the chemical NO3 radical source was characterized using UV-VIS and FT-IR spectroscopy. The amount of gas-phase NO3 radicals measured at elevated humidities was less than expected. Instead, a rise of the gas-phase HNO3 concentration was found indicating a conversion of gas-phase NO3 radicals to gas-phase HNO3 on the moist reactor walls.  相似文献   

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