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1.
Five aromatic hydrocarbons – benzene, toluene, ethylbenzene, p-xylene and 1,2,4-trimethylbenzene – were selected to investigate the laser desorption/ionization mass spectra of secondary organic aerosols (SOA) resulting from OH-initiated photooxidation of aromatic compounds. The experiments were conducted by irradiating aromatic hydrocarbon/CH3ONO/NO X mixtures in a home-made smog chamber. The aerosol time-of-flight mass spectrometer (ATOFMS) was used to measure the aerodynamic size and chemical composition of individual secondary organic aerosol particles in real-time. Experimental results showed that aerosol created by aromatics photooxidation is predominantly in the form of fine particles, which have diameters less than 2.5 μm (i.e. PM2.5), and different aromatic hydrocarbons SOA mass spectra have eight same positive laser desorption/ionization mass spectra peaks: m/z = 18, 29, 43, 44, 46, 57, 67, 77. These mass spectra peaks may come from the fragment ions of the SOA products: oxo-carboxylic acids, aldehydes and ketones, nitrogenated organic compounds, furanoid and aromatic compounds. The possible reaction mechanisms leading to these products were also discussed.  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.
Results of our aerosol study, performed during 1983–1984 in Beijing, demonstrate that ambient carbonaceous aerosols are derived mainly from coal combustion. Different SO2 oxidation processes have been observed in summer and winter. The winter sulfate appears to be produced locally and associated with products of incomplete combustion.  相似文献   

4.
Aerosol dispersion in the area surrounding an existing biological treatment facility is investigated using large-eddy simulation, with the objective to investigate the applicability of computational fluid dynamics to complex real-life problems. The aerosol sources consist of two large aeration ponds that slowly diffuse aerosols into the atmosphere. These sources are modelled as dilute concentrations of a non-buoyant non-reacting pollutant diffusing from two horizontal surfaces. The time frame of the aerosol release is restricted to the order of minutes, justifying a statistically steady inlet boundary condition. The numerical results are compared to wind-tunnel experiments for validation. The wind-tunnel flow characteristics resemble neutral atmospheric conditions with a Reynolds number, based on the boundary-layer thickness, of Re δ ≈ 2 × 105. The numerical inflow conditions are based upon the wind-tunnel flow field. The predicted decay of both the mean and root-mean-square concentrations are in good agreement with experimental data; at 3 m from the ground, the plume mean concentration 200 m downwind of the source is approximately 2% of the source strength. The numerical data in the near-surface layer (0–50 m from the ground) correspond particularly well with the wind-tunnel data. Tentative deposition simulations suggest that there seems to be little difference in the deposition rates of large (1.8 × 10−5 m) and small (3 × 10−6 m) particles in the near-field under the flow conditions considered.  相似文献   

5.
Daily measurements of atmospheric aerosol characteristics were carried out in Dolgoprudny (Moscow region) in June–August 2010. The particle concentrations at 11 size gradations within the range of 0.01–10 μm and the concentrations of cloud condensation nuclei active at water vapor supersaturation of 0.2–1% were determined. It is shown that the long anticyclonic conditions and the burning of forests and peat bogs resulted in the increase in total aerosol concentration in surface air by more than 1.5 times and in concentrations of particles with the diameter of 0.1–1 μm and > 1 μm by 5 and 10 times, respectively. The fire smoke mainly consisted of the particles with the size of 0.1–3 μm. The particles with the size of more than 5 μm were not observed. The recurrent visibility decrease up to hundreds of meters was caused by the increase in the concentration of particles with the diameter of more than 0.32μm in the air. During the smoke blanketing, the concentration of active condensation nuclei in aerosol increased almost by 20 times that created an opportunity for watering of aerosol particles and formation of the acid smog.  相似文献   

6.
Reader  M. C.  Boer  G. J. 《Climate Dynamics》1998,14(7-8):593-607
 The Canadian Centre for Climate Modelling and Analysis (CCCma) second generation climate model (GCMII) consists of an atmospheric GCM coupled to mixed layer ocean. It is used to investigate the climate response to a doubling of the CO2 concentration together with the direct effect of scattering by sulphate aerosols. As expected, the aerosols offset some of the greenhouse gas (GHG) warming; the global annual mean screen temperature change due to doubled CO2 is 3.4 °C in this model and this is reduced to 2.7 °C when an estimate of the direct effect of anthropogenic sulphate aerosols is included. The pattern of climate response to the comparatively localized aerosol forcing is not itself localized, and it bears a striking resemblance to the response pattern that arises from the globally distributed change in GHG forcing. This “non-local” response to “localized” forcing indicates that the pattern of climate response is determined, to first order, by the overall magnitude of the change in forcing rather than its detailed nature or structure. Feedback processes operating in the system apparently determine this pattern by locally amplifying and suppressing the response to the magnitude of the change in forcing. The influence of the location of the change in forcing is relatively small. These “non-local” and “local” effects of aerosol forcing are characterized and displayed and some of their consequences discussed. Effects on the moisture budget and on the energetics of the global climate are also examined. Received: 10 June 1997 / Accepted: 8 January 1998  相似文献   

7.
This paper deals with the atmospheric concentrations of PM5 and PM2.5 particulate matter and its water soluble constituents along with the size distribution of ions and spatial variation at three different residential environments in a semiarid region in India. Samples were collected from the indoors and outdoors of urban, rural and roadside sites of Agra during October 2007–March 2008. The mean concentrations of PM2.5 indoors and outdoors were 178 μgm−3 and 195 μgm−3 while the mean concentrations of PM5 indoors and outdoors were 231.8 μgm−3 and 265.2 μgm−3 respectively. Out of the total aerosol mass, water soluble constituents contributed an average of 80% (33% anions, 50% cations) in PM5 and 70% (29% anions, 43% cations) in PM2.5. The indoor–outdoor ratio of water soluble components suggested additional aerosol indoor sources at rural and roadside sites. Indoor–outdoor correlations were also determined which show poor relationships among concentrations of aerosol ions at all three sites. Univariate Pearson correlation coefficients among water soluble aerosols were determined to evaluate the relationship between aerosol ions in indoor and outdoor air.  相似文献   

8.
A continuous measurement of number size distributions and chemical composition of aerosol particles was conducted in Beijing in a dust storm event during 21-26 March 2001. The number concentration of coarse particles （ 〉2μm） increased more significantly than fine particles （ 〈2μm） during the dust storm due to dust weather, while the anthropogenic aerosols collected during the non-dust-storm period tended to be associated with fine particles. Elemental compositions were analyzed by using proton-induced X-ray emission （PIXE）. The results show that 20 elements in the dust storm were much higher than in the non-dust-storm period. The calculated soil dust concentration during the dust storm was, on average, 251.8μg m^-3, while it was only 52.1μg m^-3 on non-dust-storm days. The enrichment factors for Mg, A1, P, K, Ca, Ti, Mn, Fe, C1, Cu, Pb, and Zn show small variations between the dust storm and the non-dust-storm period, while those for Ca, Ni and Cr in the dust storm were much lower than those in the non-dust-storm period due to significant local emission sources. A high concentration and enrichment factor for S were observed during the dust storm, which implies that the dust particles were contaminated by aerosol particles from anthropogenic emissions during the long-range transport. A statistical analysis shows that the elemental composition of particles collected during the dust storm in Beijing were better correlated with those of desert soil colleted from desert regions in Inner Mongolia. Air mass back-trajectory analysis further confirmed that this dust storm event could be identified as streaks of dust plumes originating from Inner Mongolia.  相似文献   

9.
Height, time, and latitude dependences are analyzed of zonal mean vertical component of wind velocity for the period of 1992–2006 from the UKMO atmospheric general circulation model. It is shown that the ascending wind speed can provide vertical transport, against gravity, of rather large (up to 3–5μm) aerosol particles with density to 1.0–1.5 g/cm3 in the stratosphere and mesosphere. The wind velocity vertical component is supposedly a significant factor of particle motion up to 30–40–km levels and can affect sedimentation rate and residence time of the aerosol particles in the stratosphere. Structure of the mean vertical component of wind velocity allows occurrence of dynamically stable aerosol layers in the middle stratosphere.  相似文献   

10.
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   

11.
Summary The qualitative agreement of two climate models, HADCM2 and ECHAM3, on the response of surface climate to anthropogenic climate forcing in the period 2020 – 2049 is studied. Special attention is paid to the role of internal climate variability as a source of intermodel disagreement. After illustrating the methods in an intermodel comparison of simulated changes in June–August mean precipitation, some global statistics are presented. Excluding surface air temperature, the four-season mean proportion of areas in which the two models agree on the sign of the climatic response is only 53 – 60% both for increases in CO2 alone and for increases in CO2 together with direct radiative forcing by sulphate aerosols, but somewhat larger, 59 – 70% for the separate aerosol effect. In areas where the response is strong (at least twice the standard error associated with internal variability) in both models, the agreement is better and the contrast between the different forcings becomes more marked. The proportion of agreement in such areas is 57 – 75% for the response to increases in CO2 alone, 64 – 84% for the response to combined CO2 and aerosol forcing, and as high as 88 – 94% for the separate aerosol effect. The relatively good intermodel agreement for aerosol-induced climate changes is suggested to be associated with the uneven horizontal distribution of aerosol forcing. Received December 2, 1998 Revised May 5, 1999  相似文献   

12.
The seasonal variations of the concentration of particles of different sizes in the atmospheric surface layer are studied on the basis of the data of daily measurements of atmospheric aerosol characteristics in the town of Dolgoprudny (20 km from the center of Moscow) carried out in 2006–2009. It is revealed that the steady variations of monthly mean aerosol concentration are observed within the particle diameter interval of 0.02–1 μm. The annual course of concentration of these particles has two maxima, in February-March and in September–October, and one minimum in June. The concentrations of particles with the size of 0.01–0.02 μm defined by the general atmospheric background and the concentrations of particles of >1 μm associated with the local sources do not have clearly pronounced seasonal variations. It is shown that the regularities of the annual concentration variations of particles with the size of 0.02–1 μm are mainly explained by the sign and value of the lapse rate in the layer up to 925 hPa that indicates the prevalence of the vertical mixing in the processes of aerosol scattering in the surface layer as compared with the horizontal transfer.  相似文献   

13.
In this study, a regional air quality model system (RAQMS) was applied to investigate the spatial distributions and seasonal variations of atmospheric aerosols in 2006 over East Asia. Model validations demonstrated that RAQMS was able to reproduce the evolution processes of aerosol components reasonably well. Ground-level PM10 (particles with aerodynamic diameter ≤10 μm) concentrations were highest in spring and lowest in summer and were characterized by three maximum centers: the Taklimakan Desert (～1000 μg m-3), the Gobi Desert (～400 μg m-3), and the Huabei Plain (～300 μm-3) of China. Vertically, high PM10 concentrations ranging from 100 μg m-3 to 250 μg m-3 occurred from the surface to an altitude of 6000 m at 30o--45oN in spring. In winter, the vertical gradient was so large that most aerosols were restricted in the boundary layer. Both sulfate and ammonium reached their highest concentrations in autumn, while nitrate reached its maximum level in winter. Black carbon and organic carbon aerosol concentrations reached maximums in winter. Soil dust were strongest in spring, whereas sea salt exerted the strongest influence on the coastal regions of eastern China in summer. The estimated burden of anthropogenic aerosols was largest in winter (1621 Gg) and smallest in summer (1040 Gg). The sulfate burden accounted for ～42% of the total anthropogenic aerosol burden. The dust burden was about twice the anthropogenic aerosol burden, implying the potentially important impacts of the natural aerosols on air quality and climate over East Asia.  相似文献   

14.
We report on field observations in January 2009 (austral summer) of atmospheric dust devils in the northern part of the Atacama Desert in South America (≈20◦S). An extremely high level of dust-devil activity over the study site has been observed, dependent on local meteorological conditions. We found a high correlation between the dust-devil frequency of occurrence and the Obukhov length scale, L, calculated from meteorological gradient measurements, with a clear tendency for this frequency to increase with decreasing −L. The upper threshold values of −L ≈ 20–30 m, and the 2-m mean wind speed, V 2 ≈ 8m s−1, for dust-devil occurrence have been found, but the minimal V 2 threshold was not observed. Parallel routine meteorological measurements enabled us to calculate the main constituents of the surface energy balance, to obtain direct estimates of the surface albedo (α ≈ 0.21 at the solar noon) and to summarize the local conditions.  相似文献   

15.
Outdoor smog chamber experiments were performed to investigate gas/particle (G/P) partitioning behavior of aldehyde compounds in atmospheric acidic aerosols. Diesel soot and wood smoke aerosols were selected as acidic aerosols and octanal, decanal, undecanal, and cis-pinonaldehyde for aldehydes compounds. Aerosol acidity was measured with the equivalent sulfuric acid amounts in aerosol mass: 0.2–0.6 wt% in diesel soot and 0.04–0.1 wt% in wood smoke aerosols. Experimentally determined partitioning coefficients of aldehyde along with other classes of semivolatile organic compounds (SOCs) were compared with the estimation. All experimental G/P partitioning coefficients of aldehyde compounds were 10–200 times higher than estimated partitioning coefficients. Aldehyde partitioning coefficients in wood soot were similar or less than diesel soot aerosols.  相似文献   

16.
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   

17.
Water-soluble dicarboxylic acids (DCAs), ketoacids, and α-dicarbonyls in the marine aerosol samples collected over the Southern Ocean and western Pacific Ocean were determined. Oxalic acid was the most abundant species, followed by malonic acid and then succinic acid. It is suggested that aerosol concentrations of the organics over the Southern Ocean in this work represent their global background levels. Over the Southern Ocean, total concentrations of DCAs ranged from 2.9 to 7.2 ng m−3 (average: 4.5 ng m−3), ketoacids from 0.14 to 0.40 ng m−3 (av.: 0.28 ng m−3), and dicarbonyls from 0.06 to 0.29 ng m−3 (av.: 0.11 ng m−3). Over the western Pacific, total concentrations of DCAs ranged from 1.7 to 170 ng m−3 (av.: 60 ng m−3), ketoacids from 0.08 to 5.3 ng m−3 (av.: 1.8 ng m−3), and dicarbonyls from 0.03 to 4.6 ng m−3 (av.: 0.95 ng m−3). DCAs over the western Pacific have constituted a large fraction of organic aerosols with a mean DCAs-C/TC (total carbon) of 7.0% (range: 0.59–14%). Such a high value was in contrast to the low DCAs-C/TC (av.: 1.8%; range: 0.89–4.0%) for the Southern Ocean aerosols. Based on the relative abundances and latitudinal distributions of these organics, we propose that long-range atmospheric transport is more important over the western Pacific Ocean, in contrast, in situ photochemical production is more significant over the Southern Ocean although absolute concentrations of the organics are much lower.  相似文献   

18.
The effect of UV-visible light and natural sunlight on the Fe(III)-catalyzed oxidation of dissolved sulfur dioxide has been studied under the conditions representative for those of acidified atmospheric liquids. The experimental results have shown that both sunlight and UV-visible light enhance the rate of Fe(III)-catalyzed oxidation of aqueous sulfite with wavelength ranging from 300 to 575 nm. The light enhanced oxidation is mainly due to photochemical formation of OH radicals from Fe(OH)2+ complexes in the wavelength region below 420 nm and SO3•− free radicals from Fe(III) sulfite complexes above 420 nm in the absence of organic ligands. Like the Fe(III)-catalyzed thermal chemical oxidation, the Fe(III)-catalyzed photochemical oxidation is also first order with respect to sulfite ion concentration. The sunlight irradiation can increase the Fe(III)-catalyzed oxidation of S(IV) over 45%. The presence of organic complex ligands, such as oxalate, can completely inhibit the Fe-catalyzed oxidation of S(IV) in the dark. However, the photolysis of Fe(III)-oxalato complexes generates oxalate free radicals, leading to the formation of H2O2 and OH radicals and the oxidation of S(IV). The rate of Fe(III)-catalyzed oxidation of S(IV) species is found to increase with increasing light intensity. The effects of sunlight on the Fe(III)-catalyzed oxidation of S(IV) should be taken into account when predicting the daytime rates of sulfuric acid formation in atmospheric water droplets.  相似文献   

19.
This study examines the processes controlling the diurnal variability of ozone (O3) in the marine boundary layer of the Kwajalein Atoll, Republic of the Marshall Islands (latitude 8° 43′ N, longitude 167° 44′ E), during July to September 1999. At the study site, situated in the equatorial Pacific Ocean, O3 mixing ratios remained low, with an overall average of 9–10 parts per billion on a volume basis (ppbv) and a standard deviation of 2.5 ppbv. In the absence of convective storms, daily O3 mixing ratios decreased after sunrise and reached minimum during the afternoon in response to photochemical reactions. The peak-to-peak amplitude of O3 diurnal variation was approximately 1–3 ppbv. During the daytime, O3 photolysis, hydroperoxyl radicals, hydroxyl radicals, and bromine atoms contributed to the destruction of O3, which explained the observed minimum O3 levels observed in the afternoon. The entrainment of O3-richer air from the free troposphere to the local marine boundary layer provided a recovery mechanism of surface O3 mixing ratio with a transport rate of 0.04 to 0.2 ppbv per hour during nighttime. In the presence of convection, downward transport of O3-richer tropospheric air increased surface O3 mixing ratios by 3–12 ppbv. The magnitude of O3 increase due to moist convection was lower than that observed over the continent (as high as 20–30 ppbv). Differences were ascribed to the higher O3 levels in the continental troposphere and weaker convection over the ocean. Present results suggest that moist convection plays a role in surface-level O3 dynamics in the tropical marine boundary layer.  相似文献   

20.
A study has been carried out on water soluble ions, trace elements, as well as PM2.5 and PM2.5–10 elemental and organic carbon samples collected daily from Central Taiwan over a one year period in 2005. A source apportionment study was performed, employing a Gaussian trajectory transfer coefficient model (GTx) to the results from 141 sets of PM2.5 and PM2.5–10 samples. Two different types of PM10 episodes, local pollution (LOP) and Asian dust storm (ADS) were observed in this study. The results revealed that relative high concentrations of secondary aerosols (NO3−, SO42− and NH4+) and the elements Cu, Zn, Cd, Pb and As were observed in PM2.5 during LOP periods. However, sea salt species (Na+ and Cl−) and crustal elements (e.g., Al, Fe, Mg, K, Ca and Ti) of PM2.5–10 showed a sharp increase during ADS periods. Anthropogenic source metals, Cu, Zn, Cd, Pb and As, as well as coarse nitrate also increased with ADS episodes. Moreover, reconstruction of aerosol compositions revealed that soil of PM2.5–10 elevated approximately 12–14% in ADS periods than LOP and Clear periods. A significantly high ratio of non-sea salt sulfate to elemental carbon (NSS-SO42−/EC) of PM2.5–10 during ADS periods was associated with higher concentrations of non-sea-salt sulfates from the industrial regions of China. Source apportionment analysis showed that 39% of PM10, 25% of PM2.5, 50% of PM2.5–10, 42% of sulfate and 30% of nitrate were attributable to the long range transport during ADS periods, respectively.  相似文献   

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