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1.
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   

2.
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   

3.
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   

4.
In this experimental study, rate constants were measured for the reactions of ozone with 13 polycyclic aromatic hydrocarbons (PAHs) adsorbed on different types of particles. Graphite and silica were chosen to model, respectively, carbonaceous and mineral atmospheric particles. The pseudo-first order rate constants were obtained from the fit of the experimental decay of particulate PAH concentrations versus time. Second order rate constants were calculated considering the ozone gaseous concentration. At room temperature, rate constants varied, in the case of graphite particles, between (1.5 ± 0.5) × 10−17 and (1.3 ± 0.7) × 10−16 cm3 molecule−1 s−1 for chrysene and dibenzo[a,l]pyrene, respectively, and, in the case of silica particles, between (1.5 ± 0.3) × 10−17 and (1.4 ± 0.3) × 10−16 cm3 molecule−1 s−1 for fluoranthene and benzo[a]pyrene, respectively. Different granulometric parameters (particle size, pore size) and different PAH concentrations were tested in the case of silica particles. Heterogeneous reactions of ozone with particulate PAHs are shown to be more rapid than those occurring in the gas-phase, and may be competitive with atmospheric photodegradation.  相似文献   

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

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.
The precipitation events (n = 91), collected for 3 years (2000–2002) during the period of SW-monsoon (Jun–Aug) from an urban site (Ahmedabad, 23.0°N, 72.6°E) of a semi-arid region in western India, are found to exhibit characteristic differences in terms of their solute contents. The low solute (<700 μeq L−1) events are either marked by heavy precipitation amount or successive events collected during an extended rain spell; whereas light precipitation events occurring after antecedent dry period are characterized by high solutes (>700 μeq L−1). The ionic composition of low solute events show large variability due to varying contribution of anthropogenic species (: 1%–74%; : 1%–25%; and : 8%–68%) to the respective ion balance. In high solute events, ionic abundances are dominated by mineral dust (Ca2+ and ) and sea-salts (Na+ and Cl−). These differences are also reflected in the pH of low solute events (range: 5.2–7.4, VWM: 6.4) and high solute events (range: 6.6–8.2, VWM: 7.3). The comparison of Ca2+/Na+ and nss- ratios (on equivalent basis) in rain and aerosols suggests that the ionic composition of high solute events is influenced by below-cloud scavenging; whereas evidence for in-cloud scavenging is significantly reflected in low solute events. The annual wet-deposition fluxes of and are 330 and 480 mg m−2 y−1, respectively, in contrast to their corresponding dry-deposition fluxes (14 and 160 mg m−2 y−1); whereas wet and dry removal of Ca2+, Mg2+ and are comparable.  相似文献   

8.
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   

9.
The atmospheric processing by ozone of peptide-containing mixed particles was investigated as proxies for biogenic and sea spray primary organic aerosol. Reactions were performed in a flow reactor and particle composition was monitored by photoelectron resonance capture ionization aerosol mass spectrometry. Mixed particles containing dipeptides in a saturated organic matrix of stearic and palmitic acids showed no reaction under ozonolysis at exposure levels of 2.5 × 10−4 atm s O3. However reactions of mixed particles of a dipeptide (Leu-Leu) in an unsaturated matrix (oleic acid) under the same conditions resulted in a rapid loss of the peptide ion signal, as well as the carrier matrix, and appearance of a number of ion signals corresponding to secondary products. High molecular weight imides and amides have been identified corresponding to possible reactions of ozonolysis products and reactive intermediates (i.e. aldehydes, stabilized Criegee intermediates). Additionally, tautomerisation of the imides to enamines in the particle phase is postulated, with ozonolysis of the enamine followed by regioselective decomposition of the primary ozonide to form an amide whereby the peptide incorporates an aldehydic group at the N-terminus. The same general reactivity pattern was observed for mixed particles of diglycine and oleic acid. This behavior was not observed in solution phase experiments, where the tautomerisation favors the more stable imine form, indicating that particulate phase reactions of this nature may be dependent on the specific particle physical properties. The implications of this chemistry with respect the atmospheric aging of cell-derived organic aerosol are discussed.  相似文献   

10.
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   

11.
Concentrations of manganese in 56 rain events in Wilmington, NC, USA rainwater from April 1, 2005 to March 31, 2006 were 11 ± 3 nM for dissolved Mn and 1.2 ± 0.4 nM for particulate Mn. Concentrations of both forms of Mn were higher in terrestrial storms relative to marine events. This observation along with the positive correlation of Mn with pollutant indicators suggests anthropogenic inputs to rain at this location, as has been observed at other locations. The ratio of Mnpart/Mndiss was threefold larger in summer relative to winter rain, which matched the increase of particulate to dissolved Fe in rainwater suggesting influence of Saharan dust during the summer. Like Fe in rain, Mn undergoes photoreduction in rainwater, which has also been shown to be important in Mn cycling in seawater. The flux of Mn removed from the atmosphere via wet deposition is 1.5 × 10−5 moles m−2 yr−1 at this location, which is approximately twice the flux reported from two rainwater studies conducted in the early 1980s on Bermuda. Atmospheric input of Mn to the oceans is important because Mn like Fe is an essential and potentially limiting nutrient. Experiments mixing authentic rainwater and seawater demonstrate that rainwater dissolved Mn does not rapidly precipitate in seawater suggesting wet deposition is an important source of soluble, stable Mn to surface seawater.  相似文献   

12.
Ambient respirable particles (PM10; aerodynamic diameter ≤10 μm) collected in a tropical urban environment (Delhi, India) during December 2008-November 2009 were characterized with respect to 16 US EPA priority polycyclic aromatic hydrocarbons (PAHs) and 8 major and trace metals (Fe, Mn, Cd, Cu, Ni, Pb, Zn and Cr). Concentrations of Σ16PAHs (annual mean: 74.7 ± 50.7 ng m−3, range 22.1–258.4 ng m−3) and most metallic species were at least an order of magnitude greater than values reported from similar locations worldwide. Seasonal variations in Σ16PAHs were significant (p < 0.001) with highest levels in winter while crustal and anthropogenic metals showed significant but mutually opposite seasonal dependence. Statistically significant associations were observed between chemical species and various meteorological parameters. The PAH profile was dominated by combustion-derived large-ring species (~85%) that were essentially local in origin. Principal component analysis–multiple linear regression (PCA-MLR) apportioned four sources: crustal dust (73%), vehicular emission (21%), coal combustion (4%) and industrial emission (2%) that was further validated by hierarchical cluster analysis (HCA). Temporal trend analysis showed that crustal sources were predominant in summer (p < 0.05) while the remaining sources were most active in winter. Summertime intrusions of Saharan dust were identified with the help of aerosol maps and air parcel backward trajectories. Inhalation cancer risk assessment showed that up to 3,907 excess cancer cases (357 for PAHs, 122 for Cd, 2040 for Cr (VI) and 1387 for Ni) are likely in Delhi considering lifetime inhalation exposure to these chemicals at their current concentrations.  相似文献   

13.
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   

14.
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   

15.
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   

16.
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   

17.
Summary.  Mesoscale convective precipitation systems in the Alpine region are studied by analyzing radar and rain gauge data. The data from weather radars in Austria, France, Germany, and Switzerland are combined into a composite. Availability of radar data restricts the study mainly to the northern part of the Alpine region. Mesoscale convective systems (MCS) occur often in this region and are comparable to large systems observed in the USA. Seven precipitation events lasting one to six days from the years 1992–1996 are examined in detail. They all moved west to east and showed no diurnal preference in formation or dissipation. They reach sizes of 2 − 6 · 104 km2. MCS with leading-line trailing-stratiform structure tended to be larger and more intense. A 25-year set of rain gauge data indicates that a giant MCS (covering more than 4 · 104 km2 with more than 30 mm/day) occurs every 6 years in the northern Alpine region. MCS occur more frequently in the southern Alpine region. Received February 25, 1999/Revised June 29, 1999  相似文献   

18.
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   

19.
The uptake of water vapor on MgCl2×6H2O and NaCl salt dry solid films was studied over the temperature range 240 to 340 K and at 1 Torr pressure of helium using a flow reactor coupled to a modulated molecular beam mass spectrometer. The H2O to salt uptake data were obtained from the kinetics of H2O loss on salt coated Pyrex rods. The following Arrhenius expression was obtained for the initial uptake coefficient of H2O on MgCl2×6H2O films: γ 0 (MgCl2) = (6.5 ± 1.0) × 10−6 exp[(470 ± 40)/T] (calculated with specific BET surface area, quoted uncertainties are 1σ statistical). The rate of H2O adsorption on NaCl was found to be much lower than on MgCl2×6H2O, and only an upper limit was determined for the corresponding uptake coefficient: γ (NaCl) ≤ 5.6 × 10−6 at T = 300 K. The results show that the rate of H2O adsorption to salt surfaces is drastically dependent on the salt sample composition.  相似文献   

20.

Size-segregated aerosol particles were collected using a high volume MOUDI sampler at a coastal urban site in Xiamen Bay, China, from March 2018 to June 2020 to examine the seasonal characteristics of aerosol and water-soluble inorganic ions (WSIIs) and the dry deposition of nitrogen species. During the study period, the annual average concentrations of PM1, PM2.5, PM10, and TSP were 14.8?±?5.6, 21.1?±?9.0, 35.4?±?14.2 μg m?3, and 45.2?±?21.3 μg m?3, respectively. The seasonal variations of aerosol concentrations were impacted by the monsoon with the lowest value in summer and the higher values in other seasons. For WSIIs, the annual average concentrations were 6.3?±?3.3, 2.1?±?1.2, 3.3?±?1.5, and 1.6?±?0.8 μg m?3 in PM1, PM1-2.5, PM2.5–10, and PM>10, respectively. In addition, pronounced seasonal variations of WSIIs in PM1 and PM1-2.5 were observed, with the highest concentration in spring-winter and the lowest in summer. The size distribution showed that SO42?, NH4+ and K+ were consistently present in the submicron particles while Ca2+, Mg2+, Na+ and Cl? mainly accumulated in the size range of 2.5–10 μm, reflecting their different dominant sources. In spring, fall and winter, a bimodal distribution of NO3? was observed with one peak at 2.5–10 μm and another peak at 0.44–1 μm. In summer, however, the fine mode peak disappeared, likely due to the unfavorable conditions for the formation of NH4NO3. For NH4+ and SO42?, their dominant peak at 0.25–0.44 μm in summer and fall shifted to 0.44–1 μm in spring and winter. Although the concentration of NO3–N was lower than NH4–N, the dry deposition flux of NO3–N (35.77?±?24.49 μmol N m?2 d?1) was much higher than that of NH4–N (10.95?±?11.89 μmol N m?2 d?1), mainly due to the larger deposition velocities of NO3–N. The contribution of sea-salt particles to the total particulate inorganic N deposition was estimated to be 23.9—52.8%. Dry deposition of particulate inorganic N accounted for 0.95% of other terrestrial N influxes. The annual total N deposition can create a new productivity of 3.55 mgC m?2 d?1, accounting for 1.3–4.7% of the primary productivity in Xiamen Bay. In light of these results, atmospheric N deposition could have a significant influence on biogeochemistry cycle of nutrients with respect to projected increase of anthropogenic emissions from mobile sources in coastal region.

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