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1.
In this study bulk airborne aerosol composition measured by the PILS-IC (integration time of 3 min 24 s) during TRACE-P P3B Flight 10 are used to investigate the ionic chemical composition and mixing state of biomass burning particles. A biomass burning plume, roughly 3–4 days old, moderately influenced by urban pollution aerosols recorded in the Philippine Sea is investigated. Focusing on the fine particle NO3, SO42−, K+, NH4+, and water-soluble organics, the observed correlations and nearly 1-to-1 molar ratios between K+ and NO3 and between NH4+ and (SO42−+ inferred Organics) suggest the presence of fine-mode KNO3, (NH4)2SO4, and NH4(Organics) aerosols. Under the assumption that these ion pairs existed, and because KNO3 is thermodynamically less favored than K2SO4 in a mixture of NO3, SO42−, K+, NH4+, and Organic anions, the measurements suggest that aerosols could be composed of biomass burning particles (KNO3) mixed to a large degree externally with the (NH4)2SO4 aerosols. A “closed-mode” thermodynamic aerosol simulation predicts that a degree of external mixing (by SO42− mass) of 60 to 100% is necessary to achieve the observed ionic associations in terms of the existence of KNO3. However, the degree of external mixing is most likely larger than 90%, based on both the presence of KNO3 and the amounts of NH4NO3. Calculations are also shown that the aerosol mixing state significantly impacts particle growth by water condensation/evaporation. In the case of P3B Flight #10, the internal mixture is generally more hygroscopic than the external mixture. This method for estimating particle mixing state from bulk aerosol data is less definitive than single particle analysis, but because the data are quantitative, it may provide a complementary method to single particle chemical analysis.  相似文献   

2.
(NH4)2SO4, CaCl2, Na2SiO3 and NaNO3 were selected as surrogates of inorganic seed aerosols of ambient atmosphere of Chinese urban areas, respectively, to study their effects on the formation of secondary organic aerosol (SOA) in the toluene/CH3ONO/NOx photooxidation system. The SMPS and aerosol laser time-of-flight mass spectrometer (ALTOFMS) was used to measure the aerodynamic size and chemical composition of individual SOA particles in real-time. Experimental results indicate that either the growth or products of SOA is affected by the presence of inorganic seed aerosol. Inorganic seed aerosols would promote growth rates of SOA formation at the start of the reaction and inhibits its formation rate with prolonging the reaction time. In the case of about 100 μg m?3 seed aerosol load, the addition of Na2SiO3 induced a same growth rate of SOA formation as NaNO3. The influence of four individual seed aerosols on the generation of SOA decreased in the order of CaCl2 > (NH4)2SO4 > NaNO3, Na2SiO3. The presence of Na2SiO3 or NaNO3 has no obvious effect on the growth rates of SOA formation, but it does increase the yield of organic acid and nitrogen-containing organic compounds, respectively. Besides the significantly effect on the growth rate of SOA formation, the presence of CaCl2 or (NH4)2SO4 can lead to the formation of high-molecular weight species which is found to be positively correlated with the hygroscopic behavior of seed aerosols. The CaCl2 shows the strongest hygroscopic behavior among the four individual seed aerosols, and the most significant promotion effect on the formation of the high-molecular weight species. It is proposed that the SOA generation enhancement and high-molecular weight products are achieved by particle-phase heterogeneous reactions induced and catalyzed by the acidity of CaCl2 and (NH4)2SO4 seed aerosols.  相似文献   

3.
To characterize atmospheric particulate matter equal or less than 2.5 μm in diameter (PM2.5) over the Tropical Atlantic Ocean, aerosol sampling was carried out in Puerto Rico during August and September, 2006. Aerosols were analyzed by ion chromatography for water-soluble inorganic and organic ions (including Na+, NH4 +, Mg2+, Ca2+, K+, Cl?, SO4 2?, NH4 +, F?, methanesulfonate (MSA), and oxalate), by inductive coupled plasma mass spectrometry (ICPMS) for trace elements (Al, Fe, Zn, Mn, Cu, Ni, V, Pb, Cr, Sb, Co, Sc, Cd), and by scanning electron microscopy for individual aerosol particle composition and morphology. The results show that the dominant cations in aerosols were Na+, (mean: 631 ng m?3), accounting for 63.8 % of the total cation and NH4 + (mean: 164 ng m?3), accounting for 13.8 % of the total cation measured in this study. The main inorganic anions were Cl? (576 ng m?3, 54.1 %) and SO4 2? (596 ng m?3, 38.0 %). The main organic anion was oxalate (18 ng m?3). Crustal enrichment factor calculations identified 62 % of the trace elements measured (Cu, Ni, V, Co, Al, Mn, Fe, Sc, and Cr) with crustal origin. Single particle analysis demonstrated that 40 % of the aerosol particles examined were Cl? rich particles as sodium chloride from seawater and 34 % of the total particles were Si-rich particles, mainly in the form of aluminosilicates from dust material. Based on the combination of air-mass trajectories, cluster analysis and principal component analysis, the major sources of these PM2.5 particles include marine, Saharan dust and biomass burning from West Africa; however, volcanic emissions from the Soufriere Hills in Montserrat had significant impact on aerosol composition in this region at the time of sample collection.  相似文献   

4.
Size-differentiated concentrations of SPM, F, Cl, NO3, SO4, Na, K, Ca, Mg and NH4 in atmospheric aerosols were measured in a suburban area of Agra city during December 1992 to March 1993. Except for NH4, Cl and Na, all components were found to have a bimodal distribution. The fine fraction was dominated by NH4, K, NO3 and SO4, while Na, Ca, Mg, F and Cl contributed to the coarse fraction. Fifty-eight percent of SO4 and 67% of NO3 were found in the fine mode and the coarse mode comprised 42 and 33% of SO4 and NO3, respectively. SO4 was found to have a peak above the submicron range at 1.1 µm which has been attributed to secondary sulphate formation by heterogeneous oxidation of SO2 on alkaline particles of Ca and Mg. The total aerosol was basic in nature and dominated by the soil-derived acid neutralising components (Ca, Mg and Na).  相似文献   

5.
6.
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   

7.
An in-cloud scavenging case study of the major ions (NH4 +, SO4 2- and NO3 -) determining the cloudwater composition at a mountain site (1620 m.a.s.l.) is presented. A comparison between in-cloud measurements of the cloudwater composition, liquid water content, gas concentrations and aerosol concentrations and pre-cloud gas and aerosol concentrations yields the following results. Cloudwater concentrations resulted from scavenging of about half of the available NH3, aerosol NH4 +, aerosol NO3 -, and aerosol SO4 2-. Approximately a third of the SO2 was scavenged by the cloudwater and oxidized to SO4 2-. Cloud acidity during the first two hours of cloud interception (pH 3.24) was determined mostly by the scavenged gases (NH3, SO2, and HNO3); aerosol contributions to the acidity were found to be small. Observations of gas and aerosol concentrations at three elevations prior to several winter precipitation events indicated that NH3 concentrations are typically half (12–80 %) of the total (gas and aerosol) N (-III) concentrations. HNO3 typically is present at much lower concentrations (1–55 %) than aerosol NO3 -. Concentrations of SO2 are a substantial component of total sulfur, with concentrations averaging 60 % (14–76 %) of the total S (IV and VI).  相似文献   

8.
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   

9.
We investigated the acidity and concentrations of water-soluble ions in PM2.5 aerosol samples collected from an urban site in Beijing and a rural site in Gucheng, Hebei Province from November 2016 to January 2017 to gain an insight into the formation of secondary inorganic species. The average SO42–, NO3, and NH4+ concentrations were 8.3, 12.5, and 14.1 μg m–3, respectively, at the urban site and 14.0, 14.2, and 24.2 μg m–3, respectively, at the rural site. The nitrogen and sulfur oxidation ratios in urban Beijing were correlated with relative humidity (with correlation coefficient r = 0.79 and 0.67, respectively) and the aerosol loadings. Based on a parameterization model, we found that the rate constant of the heterogeneous reactions for SO2 on polluted days was about 10 times higher than that on clear days, suggesting that the heterogeneous reactions in the aerosol water played an essential role in haze events. The ISORROPIA II model was used to predict the aerosol pH, which had a mean (range) of 5.0 (4.9–5.2) and 5.3 (4.6–6.3) at the urban and rural site, respectively. Under the conditions with this predicted pH value, oxidation by dissolved NO2 and the hydrolysis of N2O5 may be the major heterogeneous reactions forming SO42– and NO3 in haze. We also analyzed the sensitivity of the aerosol pH to changes in the concentrations of SO42–, NO3, and NH4+ under haze conditions. The aerosol pH was more sensitive to the SO42– and NH4+ concentrations with opposing trends, than to the NO3 concentrations. The sensitivity of the pH was relatively weak overall, which was attributed to the buffering effect of NH3 partitioning.  相似文献   

10.
A global 3-D Lagrangian chemistry-transport model STOCHEM is used to describe the tropospheric distributions of four components of the secondary atmospheric aerosol: nitrate, sulphate, ammonium and organic compounds. The model describes the detailed chemistry of the formation of the acid precursors from the oxidation of SO2, DMS, NOx, NH3 and terpenes and their uptake into the aerosol. Model results are compared in some detail with the available surface observations. Comparisons are made between the global budgets and burdens found in other modelling studies. The global distributions of the total mass of secondary aerosols have been estimated for the pre-industrial, present day and 2030 emissions and large changes have been estimated in the mass fractions of the different secondary aerosol components.  相似文献   

11.
《Atmospheric Research》2007,83(3-4):663-679
The objective of this study was to investigate the correlation of visibility with chemical composition of Kaohsiung aerosols. Daytime visibility was observed around noon at two observation sites in metropolitan Kaohsiung, Taiwan in the years of 1999 and 2000. Both seasonal and diurnal variation patterns of visibility were observed in the region. Ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ionic species (Cl, NO3, SO4−2, NH4+, K+, Na+, Ca+2, and Mg+2) and carbonaceous contents (OC, EC, and TC), to characterize the chemical composition of Kaohsiung aerosols. Furthermore, a stepwise multiple linear regression model was developed to elucidate the influence of aerosol species on visibility impairments. The results showed that sulfate was the dominant species that affected both light scattering coefficient and visibility. On average, the percentage contributions of visibility degrading species to light scattering coefficient were 29% for sulfate, 28% for nitrate, 22% for total carbon, and 21% for PM2.5-remainder. An empirical regression model of visibility based on sulfate, nitrate, and relative humidity was also developed. The model showed that sulfate in PM2.5 was the most sensitive species to visibility variation, suggesting that the reduction of sulfate in PM2.5 could effectively improve the visibility of metropolitan Kaohsiung. During the investigation period, an event of Asian dusts intruded metropolitan Kaohsiung and dramatically increased the aerosol loadings, especially in the coarse particles. However, local visual air quality did not degrade accordingly during the Asian dust event because both visibility and light scattering coefficient are affected mainly by the fine particles. The results are discussed in detail in the paper.  相似文献   

12.
The objective of this study was to investigate the correlation of visibility with chemical composition of Kaohsiung aerosols. Daytime visibility was observed around noon at two observation sites in metropolitan Kaohsiung, Taiwan in the years of 1999 and 2000. Both seasonal and diurnal variation patterns of visibility were observed in the region. Ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ionic species (Cl, NO3, SO4−2, NH4+, K+, Na+, Ca+2, and Mg+2) and carbonaceous contents (OC, EC, and TC), to characterize the chemical composition of Kaohsiung aerosols. Furthermore, a stepwise multiple linear regression model was developed to elucidate the influence of aerosol species on visibility impairments. The results showed that sulfate was the dominant species that affected both light scattering coefficient and visibility. On average, the percentage contributions of visibility degrading species to light scattering coefficient were 29% for sulfate, 28% for nitrate, 22% for total carbon, and 21% for PM2.5-remainder. An empirical regression model of visibility based on sulfate, nitrate, and relative humidity was also developed. The model showed that sulfate in PM2.5 was the most sensitive species to visibility variation, suggesting that the reduction of sulfate in PM2.5 could effectively improve the visibility of metropolitan Kaohsiung. During the investigation period, an event of Asian dusts intruded metropolitan Kaohsiung and dramatically increased the aerosol loadings, especially in the coarse particles. However, local visual air quality did not degrade accordingly during the Asian dust event because both visibility and light scattering coefficient are affected mainly by the fine particles. The results are discussed in detail in the paper.  相似文献   

13.
A unified chemistry-aerosol-climate model is applied in this work to compare climate responses to chang- ing concentrations of long-lived greenhouse gases(GHGs,CO2,CH4,N2O),tropospheric O3,and aerosols during the years 1951–2000.Concentrations of sulfate,nitrate,primary organic carbon(POA),secondary organic carbon(SOA),black carbon(BC)aerosols,and tropospheric O3 for the years 1950 and 2000 are obtained a priori by coupled chemistry-aerosol-GCM simulations,and then monthly concentrations are in- terpolated ...  相似文献   

14.
A three-dimensional model of the global ammonia cycle   总被引:16,自引:0,他引:16  
Using a three-dimensional (3-D) transport model of the troposphere, we calculated the global distributions of ammonia (NH3) and ammonium (NH 4 + ), taking into account removal of NH3 on acidic aerosols, in liquid water clouds and by reaction with OH. Our estimated global 10°×10° NH3 emission inventory of 45 Tg N-NH3 yr provides a reasonable agreement between calculated wet NH 4 + deposition and measurements and of measured and modeled NH 4 + in aerosols, although in Africa and Asia especially discrepancies exist.NH3 emissions from natural continental ecosystems were calculated applying a canopy compensation point and oceanic NH3 emissions were related to those of DMS (dimethylsulfide). In many regions of the earth, the pH found in rain and cloud water can be attributed to acidity derived from NO, SO2 and DMS emissions and alkalinity from NH3. In the remote lower troposphere, sulfate aerosols are calculated to be almost neutralized to ammonium sulfate (NH4)2SO4, whereas in the middle and upper troposphere, according to our calculations, the aerosol should be more acidic, as a result of the oxidation of DMS and SO2 throughout the troposphere and removal of NH3 on acidic aerosols at lower heights. Although the removal of NH3 by reaction with the OH radical is relatively slow, the intermediate NH2 radical can provide a substantial annual N2O source of 0.9 –0.4 +0.9 Tg, thus contributing byca. 5% to estimated global N2O production. The oxidation by OH of NH3 from anthropogenic sources accounts for 10% of the estimated total anthropogenic sources of N2O. This source was not accounted for in previous studies, and is mainly located in the tropics, which have high NH3 and OH concentrations. Biomass burning plumes, containing high NO x and NH3 concentrations provide favourable conditions for gas phase N2O production. This source is probably underestimated in this model study, due to the coarse resolution of the 3-D model, and the rather low biomass burning NH3 and NO x emissions adopted. The estimate depends heavily on poorly known concentrations of NH3 (and NO x ) in the tropics, and uncertainties in the rate constants of the reactions NH2 + NO2 N2O + H2O (R4), and NH2 + O3 NH2O + O2 (R7).  相似文献   

15.
A box model, involving simple heterogeneous reaction processes associated with the production of non-sea-salt sulfate (nss-SO 4 2– ) particles, is used to investigate the oxidation processes of dimethylsulfide (DMS or CH3SCH3) in the marine atmosphere. The model is applied to chemical reactions in the atmospheric surface mixing layer, at intervals of 15 degrees latitude between 60° N and 60° S. Given that the addition reaction of the hydroxyl radical (OH) to the sulfur atom in the DMS molecule is faster at lower temperature than at higher temperature and that it is the predominant pathway for the production of methanesulfonic acid (MSA or CH3SO3H), the results can well explain both the increasing tendency of the molar ratio of MSA to nss-SO 4 2– toward higher latitudes and the uniform distribution with latitude of sulfur dioxide (SO2). The predicted production rate of MSA increases with increasing latitude due to the elevated rate constant of the addition reaction at lower temperature. Since latitudinal distributions of OH concentration and DMS reaction rate with OH are opposite, a uniform production rate of SO2 is realized over the globe. The primary sink of DMS in unpolluted air is caused by the reaction with OH. Reaction of DMS with the nitrate radical (NO3) also reduces DMS concentration but it is less important compared with that of OH. Concentrations of SO2, MSA, and nss-SO 4 2– are almost independent of NO x concentration and radiation field. If dimethylsulfoxide (DMSO or CH3S(O)CH3) is produced by the addition reaction and further converted to sulfuric acid (H2SO4) in an aqueous solution of cloud droplets, the oxidation process of DMSO might be important for the production of aerosol particles containing nss-SO 4 2– at high latitudes.  相似文献   

16.
A multifunctional HTDMA system with a robust temperature control   总被引:3,自引:0,他引:3  
The hygroscopicity of atmospheric aerosols significantly influences their size distribution, cloud condensation nuclei ability, atmospheric residence time, and climate forcing. In order to investigate the hygroscopic behavior of aerosol particles and serious haze in China, a Hygroscopic Tandem Differential Mobility Analyzers (HTDMA) system was designed and constructed at Fudan University. It can function as a scanning mobility particle sizing system to measure particle size distribution in the range of 20--1000 nm in diameter, as well as a hygroscopicity analyzer for aerosol particles with diameters between 20--400 nm in the range of 20%--90% RH (relative humidity). It can also measure the effect of uptake of inorganic acids or semi-VOCs on the hygroscopic behavior of aerosols, such as typical inorganic salts in atmospheric dust or their mixtures. The performance tests show that the system measured particle size of the standard polystyrene latex spheres (PSLs) is 197 nm, which is in excellent agreement with the certified diameter D=199±6 nm, as well as a standard deviation of the repeated runs SD=8.9x10-4. In addition, the measured hygroscopic growth factors of the model compounds, (NH4)2SO4 and NaNO3, agree with the Kohler theoretical curves. The results indicate that the HTDMA system is an excellent and powerful tool for studying the hygroscopic behavior of submicron aerosols and meets the demand required for laboratory research and fieldwork on atmospheric aerosols in China.  相似文献   

17.
The chemical compositions (Na+, NH4 +, K+, Mg2+, Ca2+, Cl?, NO2 ?, NO3 ?, SO4 2?, HCO3 ?) of wet precipitation and nitrogen isotope compositions δ15N(NH4 +) were studied from January to December 2010 in Wroc?aw (SW Poland). Results of a principle component analysis show that 82 % of the data variability can be explained by three main factors: 1) F1 (40 %) observed during vegetative season (electrical conductivity, HCO3 ?, NO3 ?, NO2 ?, NH4 + and SO4 2?), mainly controlling rainwater mineralization; 2) F2 (26 %) observed during vegetative and heating seasons (K+, Ca2+ and Mg2+), probably representing a combination of two processes: anthropogenic dusts and fertilizers application in agricultural fields, and 3) F3 (16 %) reported mainly during heating season (Na+ and Cl?) probably indicating the influence of marine aerosols. Variations of δ15N(NH4 +) from ?11.5 to 18.5?‰ identify three main pathways for the formation of NH4 +: 1) equilibrium fractionation between NH3 and NH4 +; 2) kinetic exchange between NH3 and NH4 +; 3) NH4 + exchange between atmospheric salts particles and precipitation. The coupled chemical/statistical analysis and δ15N(NH4 +) approach shows that while fossil fuels burning is the main source of NH4 + in precipitation during the heating season, during the vegetative season NH4 + originates from local sewage irrigation fields in Osobowice or agricultural fertilizers.  相似文献   

18.
The acidification of precipitation and the wet removal of pollutants in South China in spring are evaluated by using a one dimensional, time-dependent, physico-chemical model of stratiform clouds. The results are consistent with the mean field data. In the typical condition, the in-cloud scavenging of gases and aerosols is the major removal process at the begining of rainfall, then fractions of below-cloud scavenging of S(VI) from S(IV) oxidation, NH3, HNO3 and particles increase gradually. It can be treated as an irreversible process. Numerical tests show that the concentration of oxidants, H2O2 can affect wet removal of SO2, as well as the formation and deposition amount of S(VI). The convergence of airflow can compensate partially the depletion of pollutants by wet removal.  相似文献   

19.
台山铜鼓湾低层大气盐类气溶胶分布特征   总被引:13,自引:0,他引:13  
1989年2月在台山铜鼓湾海边对水溶性气溶胶的离子成分Cl~-、NO_3~-、SO_4~=、Na~+、K~+、Mg~(++)进行了分析,发现其中主要离子成分是Cl~-与Na~+,它们都来自海盐气溶胶,Mg~(++)亦来自海盐;而K~+主要是陆源性的;SO_~=的来源以海盐为主,但也反映出受东亚大陆较严重大面积硫污染影响的特征;而NO_3~-有较高的富集现象,且100%为非海盐成分,应是局地人类活动,如农耕与炊事影响所致。  相似文献   

20.
Industrial pollution has a significant effect on aerosol properties in Changsha City, a typical city of central China.Therefore, year-round measurements of aerosol optical, radiative and chemical properties from 2012 to 2014 at an urban site in Changsha were analyzed. During the observation period, the energy structure was continuously optimized, which was characterized by the reduction of coal combustion. The aerosol properties have obvious seasonal variations. The seasonal average aerosol opti...  相似文献   

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