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1.
Aerosol light-scattering in The Netherlands   总被引:2,自引:0,他引:2  
The relation between the (midday) aerosol light-scattering and the concentrations of nitrate and sulfate has been assessed at a site near the coast of the North Sea in The Netherlands. Midday was selected for the measurements because this is the time at which the aerosol is most effective in the scattering of solar radiation. Automated thermodenuders were used for the hourly measurement of the concentration of nitrate and sulfate with a lower detection limit of 0.1 μ m−3. The site is operational since October 1993. The first-year average dry aerosol light-scattering (measured with an integrating nephelometer at a wavelength of 525 nm) was 0.71 × 10−4 m1̄. In arctic marine air the aerosol light-scattering was a factor of 10 lower than the average value, in polluted continental air it was up to a factor of 10 higher. The ratio of the total aerosol light-scattering to the concentration of sulfate was 20 m2 g−1. The contribution of nitrate to the aerosol light-scattering was higher than that of sulfate in the winter and of about equal magnitude in the summer period. In November and December of 1993, the humidity dependence of the aerosol light-scattering was investigated. Two types of (continental) aerosol were found with respect to the humidity behavior. One type showed a significant increase in light-scattering at the deliquescence points of ammonium nitrate and ammonium sulfate, with that of ammonium nitrate the most pronounced. The second type of continental aerosol did not show deliquescence, but followed the typical humidity dependence of aerosol in a supersaturated droplet state. In this latter aerosol type, nitrate dominated over sulfate. It was concluded from the study that the aerosol light-scattering in The Netherlands, in particular its humidity dependence, is governed by (ammonium) nitrate.  相似文献   

2.
The purpose of this study is to explore the possible reasons accounting for elevated nitrate aerosol levels during high particulate days (HPD) in Taichung urban area of central Taiwan. To achieve this goal, simultaneous measurements of particulate and gaseous pollutants were carried out from September 2004 to April 2005 using an annular denuder system (ADS). The formation rate of NO2 to nitrate aerosol, calculated using the relevant chemical reactions, was employed to interpret enhanced nitrate aerosol concentrations during HPD. The observations showed that nitrate concentration during HPD was 14 times higher than that during low particulate days (LPD). The average formation rate during HPD was 4.0% h?1, which was 3.1 times higher than that during LPD. The quantitative analysis showed that the formation rate was mainly influenced by temperature and relative humidity. Lower temperature and higher relative humidity led much nitrate aerosol formation in HPD. Moreover, the residence time analysis of air masses staying over the studied area showed that the slow-motion air retained high nitrate concentrations due to more nitrate aerosol converted from the precursors in NOx-rich areas.  相似文献   

3.
In the frame of the MIUR-AEROCLOUDS project (Study of Direct and Indirect Aerosol Effects on Climate), night-time and daytime size-segregated aerosol samples were collected concurrently at five different sites (near-city, urban, rural, marine and mountain background sites). The paper reports on the daily evolution of the main aerosol chemical characteristics as a function of particle size in different environments over the Italian Peninsula, spanning from the Po Valley to the south Tyrrhenian coast.Two 4-day intensive observation periods (IOPs) were undertaken in July 2007 and February 2008, under meteorological conditions typical of the summer and winter climate for Italy.In the summer IOP, under stable atmospheric conditions, at the low-altitude continental sites the diurnal evolution of the planetary boundary layer (PBL), induces an atmospheric dilution effect driving the particulate matter (PM) concentrations, while, at the mountain site, it determines the upward motion of polluted air masses from the Po Valley PBL in daytime.The fine fraction was dominated by ammonium salts and carbonaceous matter (water-soluble organic matter, WSOM, and water-insoluble carbonaceous matter, WINCM). High concentrations of ammonium sulphate and WSOM due to enhanced photochemical activity constituted the background aerosol composition over the whole country, whereas, ammonium nitrate and WINCM were more associated to local emissions (e.g. urban site with concentrations peaking in the finest size range due to strong local traffic-related sources of ultrafine particles).During the winter IOP in the Po Valley, the shallow PBL depths and low wind velocity, especially at night, favoured the condensation of semi-volatile species (i.e. organic matter and ammonium nitrate), causing the high fine PM concentration observed at ground level.  相似文献   

4.
Atmospheric concentrations of gaseous NH3 and HNO3 and of particulate NH4+ and NO3- were measured during various seasons at a forest ecosystem research site in the "Fichtelgebirge" mountains in Central Europe. Air masses arriving at this site were highly variable with respect to trace compound concentration levels and their concentration ratios. However, the distributions of NH4+ and NO3- within the aerosol particle size spectra exhibited some very consistent patterns, with the former dominating the fine particle concentrations, and the latter dominating the coarse particles range, respectively. Overall, the particulate phase (NH4+ + NO3-) dominated the atmospheric nitrogen budget (particulate and gas phase, NH4+ + NO3- + NH3 + HNO3) by more than 90% of the median total mixing ratio in winter, and by more than 60% in summer. The phase partitioning varied significantly between the winter and summer seasons, with higher relative importance of the gaseous species during summer, when air temperatures were higher and relative humidities lower as compared to the winter season. Reduced nitrogen dominated over oxidized nitrogen, indicating the prevailing influence of emissions from agricultural activity as compared to traffic emissions at this mountainous site. A model has been successfully applied in order to test the hypothesis of thermodynamic equilibrium between the particulate and gas phases.  相似文献   

5.
Air quality data collected in the California Regional PM10/ PM(2.5) Air Quality Study (CRPAQS) are analyzed to qualitatively assess the processes affecting secondary aerosol formation in the San Joaquin Valley (SJV). This region experiences some of the highest fine particulate matter (PM(2.5)) mass concentrations in California (< or = 188 microg/m3 24-hr average), and secondary aerosol components (as a group) frequently constitute over half of the fine aerosol mass in winter. The analyses are based on 15 days of high-frequency filter and canister measurements and several months of wintertime continuous gas and aerosol measurements. The phase-partitioning of nitrogen oxide (NO(x))-related nitrogen species and carbonaceous species shows that concentrations of gaseous precursor species are far more abundant than measured secondary aerosol nitrate or estimated secondary organic aerosols. Comparisons of ammonia and nitric acid concentrations indicate that ammonium nitrate formation is limited by the availability of nitric acid rather than ammonia. Time-resolved aerosol nitrate data collected at the surface and on a 90-m tower suggest that both the daytime and nighttime nitric acid formation pathways are active, and entrainment of aerosol nitrate formed aloft at night may explain the spatial homogeneity of nitrate in the SJV. NO(x) and volatile organic compound (VOC) emissions plus background O3 levels are expected to determine NO(x) oxidation and nitric acid production rates, which currently control the ammonium nitrate levels in the SJV. Secondary organic aerosol formation is significant in winter, especially in the Fresno urban area. Formation of secondary organic aerosol is more likely limited by the rate of VOC oxidation than the availability of VOC precursors in winter.  相似文献   

6.
This paper describes the results of a study to determine the total mass and the mass distribution of atmospheric aerosols, especially that mass associated with particles greater than 10 μm diameter. This study also determined what fraction of the total aerosol mass a standard high-volume air sampler collects and what fraction and size interval settle out on a dust fall plate. A special aerosol sampling system was designed for this study to obtain representative samples of large airborne particles. A suburban sampling site was selected because no local point sources of aerosols existed nearby. Samples were collected under various conditions of wind velocity and direction to obtain measurements on different types of aerosols.

Study measurements show that atmospheric particulate matter has a bimodal mass distribution. Mass associated with large particles mainly ranged from 5 to 100 μm in size, while mass associated with small particles ranged from an estimated 0.03 to 5 μm in size. Combined, these two distributions produced a bimodal mass distribution with a minimum around 5 μm diameter. The high-volume air sampler was found to collect most of the total aerosol mass, not just that fraction normally considered suspended particulate. Dust fall plates did not provide a good or very useful measure of total aerosol mass. The two fundamental processes of aerosol formation, condensation and dispersion appear to account for the formation of a bimodal mass distribution in both natural and anthropogenic aerosols. Particle size distribution measurements frequently are in error because representative samples of large airborne particles are not obtained. Considering this descrepancy, air pollution regulations should specify or be based upon an upper particle size limit.  相似文献   

7.
The ionic compositions of particulate matter with aerodynamic diameter < or = 2.5 microm (PM2.5) and size-resolved aerosol particles were measured in Big Bend National Park, Texas, during the 1999 Big Bend Regional Aerosol and Visibility Observational study. The ionic composition of PM2.5 aerosol was dominated by sulfate (SO4(2-)) and ammonium (NH4+). Daily average SO4(2-) and NH4+ concentrations were strongly correlated (R2 = 0.94). The molar ratio of NH4+ to SO4(2-) averaged 1.54, consistent with concurrent measurements of aerosol acidity. The aerosol was observed to be comprised of a submicron fine mode consisting primarily of ammoniated SO4(2-) and a coarse particle mode containing nitrate (NO3-). The NO3- appears to be primarily associated with sea salt particles where chloride has been replaced by NO3-, although formation of calcium nitrate (Ca(NO3)2) is important, too, on several days. Size-resolved aerosol composition results reveal that a size cut in particulate matter with aerodynamic diameter < or = 1 microm would have provided a much better separation of fine and coarse aerosol modes than the standard PM2.5 size cut utilized for the study. Although considerable nitric acid exists in the gas phase at Big Bend, the aerosol is sufficiently acidic and temperatures sufficiently high that even significant future reductions in PM2.5 SO4(2-) are unlikely to be offset by formation of particulate ammonium nitrate in summer or fall.  相似文献   

8.
The Reedy River branch of Lake Greenwood, SC, has repeatedly experienced summertime algal blooms, upsetting the natural system. This lake's shallow depth makes It susceptible to atmospheric influence. A series of experiments were carried out in order to investigate the effect of atmospheric nitrogen deposition into the lake. Nitrogen was examined because of the insignificant phosphorus dry atmospheric flux and the unique nutrient demands of the dominant algae (Pithophora oedogonia) contributing to the blooms. In this paper, results are presented, of the experimental measurement of coarse and fine atmospheric concentrations of atmospheric particulate nitrogen adjacent to and in the watershed of the Reedy River (downtown Greenville) and Lake Greenwood. Experiments were carried out during four 24-hr periods in January 2001 and again during four 24-hr periods in March 2001. Results are presented here for atmospheric particulate nitrogen as well as other constituents of the airborne aerosol. Mass concentrations of PM2.5 averaged 14.0 and 21 microg/m3 for Lake Greenwood and downtown Greenville, respectively. Mass concentrations of total suspended particulates (TSP) averaged 22.6 and 38.5 microg/m3 for Lake Greenwood and downtown Greenville, respectively. This ambient aerosol concentration was apportioned to its chemical constituents, and the greatest contributors to PM2.5 mass were organics (45 and 42% for downtown Greenville and the lake, respectively) and sulfate (14.1 and 19.7% for downtown Greenville and the lake, respectively). The information gathered here, despite its episodic nature, is important not only in determining atmospheric nitrogen but also in documenting the composition of aerosol in South Carolina, which so far has not been studied. In a companion paper, results for gaseous pollutants as well as thermodynamic modeling of the aerosol and nitrogen flux determinations are presented.  相似文献   

9.
Experimental relationships between the mass concentration of suspended particulate matter and the optical density of particulates collected on paper tape have been determined for the atmospheric aerosol and for aerosols of constant optical properties. Simultaneous samples were obtained on membrane filters (for gravimetric analysis) and on Whatman No. 4 paper tape (for optical evaluation). Sampling procedures were adopted which ensured that the efficiency of sampling was the same in both cases.

Consistent relationships between mass concentrations of suspended particulate matter and optical density expressed in terms of per cent transmittance or per cent reflectance were found for dispersions of coal, limestone, fly ash, and a coal-limestone mixture.

For atmospheric aerosol samples collected on the roof of the Graduate School of Public Health, University of Pittsburgh, the relationship between mass concentration and per cent transmittance or per cent reflectance was found to be linear over the range of values observed. The correlation coefficients were ?0.93 (for concentration versus per cent transmittance) and ?0.89 (for concentration versus per cent reflectance).  相似文献   

10.
The equilibrium between gaseous ammonia, nitric acid, and aerosol nitrate is discussed on the basis of a recent field experiment in southern California. Comparison is drawn between theoretical equilibrium calculations and simultaneous measurements of nitric acid, ammonia, ammonium ion, nitrate ion, sulfate ion, other ionic species, temperature and dewpoint. Particulate and gaseous pollutant concentrations at some inland sampling sites are readily explained if the aerosol is assumed to exist as an external mixture with all particulate nitrate and ammonium available to form pure NH4NO3. At other monitoring sites, especially near the coast, aerosol nitrate is found in the presence of NH3 and HNO3 concentrations that thermodynamic calculations show are too low to produce pure NH4NO3. This can be explained when the amount of aerosol nitrate that can be derived from reaction of nitric acid with sea salt and soil dust is taken into account. A calculation approach that accounts for the presence of mixed sulfate and nitrate salts improves the agreement between predicted and observed pollutant concentrations in the majority of cases studied. Uncertainties in these calculations arise from a number of sources including the thermodynamic quantities, and the effect of these uncertainties on the comparison between theory and experiment is discussed.  相似文献   

11.
Abstract

Air quality data collected in the California Regional PM10/PM2.5 Air Quality Study (CRPAQS) are analyzed to qualitatively assess the processes affecting secondary aerosol formation in the San Joaquin Valley (SJV). This region experiences some of the highest fine particulate matter (PM2.5) mass concentrations in California (≤188 μg/m3 24-hr average), and secondary aerosol components (as a group) frequently constitute over half of the fine aerosol mass in winter. The analyses are based on 15 days of high-frequency filter and canister measurements and several months of wintertime continuous gas and aerosol measurements. The phase-partitioning of nitrogen oxide (NOx)-related nitrogen species and carbonaceous species shows that concentrations of gaseous precursor species are far more abundant than measured secondary aerosol nitrate or estimated secondary organic aerosols. Comparisons of ammonia and nitric acid concentrations indicate that ammonium nitrate formation is limited by the availability of nitric acid rather than ammonia. Time-resolved aerosol nitrate data collected at the surface and on a 90-m tower suggest that both the daytime and nighttime nitric acid formation pathways are active, and entrainment of aerosol nitrate formed aloft at night may explain the spatial homogeneity of nitrate in the SJV. NOx and volatile organic compound (VOC) emissions plus background O3 levels are expected to determine NOx oxidation and nitric acid production rates, which currently control the ammonium nitrate levels in the SJV. Secondary organic aerosol formation is significant in winter, especially in the Fresno urban area. Formation of secondary organic aerosol is more likely limited by the rate of VOC oxidation than the availability of VOC precursors in winter.  相似文献   

12.
13.
Measurements of 15-min average PM2.5 concentrations were made with a real-time light-scattering instrument at both outdoor (central monitoring sites in three communities) and indoor (residential) locations over two seasons in the Minneapolis-St. Paul metropolitan area. These data are used to examine within-day variability of PM2.5 concentrations indoors and outdoors, as well as matched indoor-to-outdoor (I/O) ratios. Concurrent gravimetric measurements of 24-hr average PM2.5 concentrations were also obtained as a way to compare real-time measures with this more traditional metric. Results indicate that (1) within-day variability for both indoor and outdoor 15-min average PM2.5 concentrations was substantial and comparable in magnitude to day-to-day variability for 24-hr average concentrations; (2) some residences exhibited substantial variability in indoor aerosol characteristics from one day to the next; (3) peak values for indoor short-term (15-min) average PM2.5 concentrations routinely exceeded 24-hr average outdoor values by factors of 3-4; and (4) relatively strong correlations existed between indoor and outdoor PM2.5 concentrations for both 24-hr and 15-min averages.  相似文献   

14.
Several collocated semicontinuous instruments measuring particulate matter with particle sizes < or =2.5 microm (PM2.5) sulfate (SO4(2-)) and nitrate (NO3-) were intercompared during two intensive field campaigns as part of the PM2.5 Technology Assessment and Characterization Study. The summer 2001 urban campaign in Queens, NY, and the summer 2002 rural campaign in upstate New York (Whiteface Mountain) hosted an operation of an Aerosol Mass Spectrometer, Ambient Particulate Sulfate and Nitrate Monitors, a Continuous Ambient Sulfate Monitor, and a Particle-Into-Liquid Sampler with Ion Chromatographs (PILS-IC). These instruments provided near real-time particulate SO4(2-) and NO3- mass concentration data, allowing the study of particulate SO4(2-)/NO3- diurnal patterns and detection of short-term events. Typical particulate SO4(2-) concentrations were comparable at both sites (ranging from 0 to 20 microg/m3), while ambient urban particulate NO3- concentrations ranged from 0 to 11 microg/m3 and rural NO3- concentration was typically less than 1 microg/m3. Results of the intercomparisons of the semicontinuous measurements are presented, as are results of the comparisons between the semicontinuous and time-integrated filter-based measurements. The comparisons at both sites, in most cases, indicated similar performance characteristics. In addition, charge balance calculations, based on major soluble ionic components of atmospheric aerosol from the PILS-IC and the filter measurements, indicated slightly acidic aerosol at both locations.  相似文献   

15.
ABSTRACT

Wintertime atmospheric light scattering in Dallas, TX, was estimated through the use of aerosol models. Input data for the aerosol models were provided by measurements of aerosol chemistry, physical particle size distributions, and distributions of particulate sulfur by particle size, and by predictions by an atmospheric simulation model. Light scattering measurements provided a basis for testing the aerosol models. The SCAPE thermodynamic equilibrium model was used to estimate the amount of liquid water associated with particles and the ELSIE Mie scattering model was applied to estimate the resulting light scattering. The calculations were based on aerosol properties measured in Dallas during December 1994 and February 1995, and changes in scattering due to hypothetical changes in the aerosol were predicted. The predicted light scattering was compared to scattering measured by an Optec nephelom-eter; agreement was within 20% in every case.  相似文献   

16.
Evaporative loss of particulate matter (with aerodynamic diameter < 2.5 microm, [PM2.5]) ammonium nitrate from quartz-fiber filters during aerosol sampling was evaluated from December 3, 1999, through February 3, 2001, at two urban (Fresno and Bakersfield) and three nonurban (Bethel Island, Sierra Nevada Foothills, and Angiola) sites in central California. Compared with total particulate nitrate, evaporative nitrate losses ranged from < 10% during cold months to > 80% during warm months. In agreement with theory, evaporative loss from quartz-fiber filters in nitric acid denuded samplers is controlled by the ambient nitric acid-to-particulate nitrate ratio, which is determined mainly by ambient temperature. Accurate estimation of nitrate volatilization requires a detailed thermodynamic model and comprehensive chemical measurements. For the 14-month average of PM2.5 acquired on Teflon-membrane filters, measured PM2.5 mass was 8-16% lower than actual PM2.5 mass owing to nitrate volatilization. For 24-hr samples, measured PM2.5 was as much as 32-44% lower than actual PM2.5 at three California Central Valley locations.  相似文献   

17.
Wintertime atmospheric light scattering in Dallas, TX, was estimated through the use of aerosol models. Input data for the aerosol models were provided by measurements of aerosol chemistry, physical particle size distributions, and distributions of particulate sulfur by particle size, and by predictions by an atmospheric simulation model. Light scattering measurements provided a basis for testing the aerosol models. The SCAPE thermodynamic equilibrium model was used to estimate the amount of liquid water associated with particles and the ELSIE Mie scattering model was applied to estimate the resulting light scattering. The calculations were based on aerosol properties measured in Dallas during December 1994 and February 1995, and changes in scattering due to hypothetical changes in the aerosol were predicted. The predicted light scattering was compared to scattering measured by an Optec nephelometer; agreement was within 20% in every case.  相似文献   

18.
Abstract

The Reedy River branch of Lake Greenwood, SC, has repeatedly experienced summertime algal blooms, upsetting the natural system. This lake’s shallow depth makes it susceptible to atmospheric influence. A series of experiments were carried out in order to investigate the effect of atmospheric nitrogen deposition into the lake. Nitrogen was examined because of the insignificant phosphorus dry atmospheric flux and the unique nutrient demands of the dominant algae (Pithophora oedogonia) contributing to the blooms.

In this paper, results are presented of the experimental measurement of coarse and fine atmospheric concentrations of atmospheric particulate nitrogen adjacent to and in the watershed of the Reedy River (downtown Greenville) and Lake Greenwood. Experiments were carried out during four 24-hr periods in January 2001 and again during four 24-hr periods in March 2001. Results are presented here for atmospheric particulate nitrogen as well as other constituents of the airborne aerosol. Mass concentrations of PM2.5 averaged 14.0 and 21 µg/m3 for Lake Greenwood and downtown Greenville, respectively. Mass concentrations of total suspended particulates (TSP) averaged 22.6 and 38.5 μg/m3 for Lake Greenwood and downtown Greenville, respectively. This ambient aerosol concentration was apportioned to its chemical constituents, and the greatest contributors to PM2.5 mass were organics (45 and 42% for downtown Greenville and the lake, respectively) and sulfate (14.1 and 19.7% for downtown Greenville and the lake, respectively).

The information gathered here, despite its episodic nature, is important not only in determining atmospheric nitrogen but also in documenting the composition of aerosol in South Carolina, which so far has not been studied. In a companion paper, results for gaseous pollutants as well as thermodynamic modeling of the aerosol and nitrogen flux determinations are presented.  相似文献   

19.
The research objective was to adapt the ultraviolet (UV)-photolysis method to determine dissolved organic nitrogen (DON) in aqueous extracts of aerosol samples. DON was assumed to be the difference in total concentration of inorganic nitrogen forms before and after sample irradiation. Using a 2(2) factorial design the authors found that the optimal conversion of urea, amino acids (alanine, aspartic acid, glycine, and serine), and methylamine for a reactor temperature of 44 degrees C occurred at pH 2.0 with a 24-hr irradiance period at concentrations <33 microM of organic nitrogen. Different decomposition mechanisms were evident: the photolysis of amino acids and methylamine released mainly ammonium (NH4+), but urea released a near equimolar ratio of NH4+ and nitrate (NO3-). The method was applied to measure DON in the extracts of aerosol samples from Tampa, FL, over a 32-day sampling period. Average dissolved inorganic (DIN) and DON concentrations in the particulate matter fraction PM10 were 78.1 +/- 29.2 nmol-Nm(-3) and 8.3 +/- 4.9 nmol-Nm(-3), respectively. The ratio between DON and total dissolved nitrogen ([TDN] = DIN + DON) was 10.1 +/- 5.7%, and the majority of the DON (79.1 +/- 18.2%) was found in the fine particulate matter (PM2.5) fraction. The average concentrations of DIN and DON in the PM2.5 fraction were 54.4 +/- 25.6 nmol-Nm(-3) and 6.5 +/- 4.4 nmol-Nm(-3), respectively.  相似文献   

20.
First-time measurements of the potentially toxic inorganic species of arsenic (arsenite arid arsenate) have been obtained in fine (<2.5 µm AD) and coarse (>2.5 µm AD) atmospheric particles in the Los Angeles area. A recently developed method that includes procedures for sample collection, preparation, and analysis was used in this study. Size-fractlonated aerosol samples were collected with a high-volume dichotomous virtual impactor that employed polytetrafluoroethylene filters. Results were obtained for the recovery of arsenic standards added to unexposed and collected filters. Data from this study, indicated that the recently developed speciation method can be used to determine concentrations of As(lll) and As(V) In atmospheric particulate matter samples.

Size-fractionated aerosol samples were collected in the city of Industry during January and February 1987. In most samples, As(lll) and As( V) were above the detection limit (approximately 1 ng m-3 of either species) in both aerosol size fractions. A greater portion (about 75 percent) of the two species were observed in the fine particles. The As(lll)/As(V) ratio for both particle sizes was close to 1 (I.e., an equal mixture of both species). Comparison of total suspended particulate arsenic measured by the speciation method to that measured by a routine California Air Resources Board-approved procedure showed good agreement (r = 0.94), indicating both methods were approximately equivalent for the collection and analysis of aerosol arsenic.  相似文献   

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