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1.
Long-term measurements of ambient particulate matter less than 2.5 μm in diameter (PM2.5) and its chemical compositions were performed at a rural site in Korea from December 2005 to August 2009. The average PM2.5 concentration was 31 μg m−3 for the whole sampling period, and showed a slightly downward annual trend. The major components of PM2.5 were organic carbon, SO42−, NO3−, and NH4+, which accounted for 55 % of total PM2.5 mass on average. For the top 10 % of PM2.5 samples, anionic constituents and trace elements clearly increased while carbonaceous constituents and NH4+ remained relatively constant. Both Asian dust and fog events clearly increased PM2.5 concentrations, but affected its chemical composition differently. While trace elements significantly increased during Asian dust events, NO3−, NH4+ and Cl were dramatically enhanced during fog events due to the formation of saturated or supersaturated salt solution. The back-trajectory based model, PSCF (Potential Source Contribution Function) identified the major industrial areas in Eastern China as the possible source areas for the high PM2.5 concentrations at the sampling site. Using factor analysis, soil, combustion processes, non-metal manufacture, and secondary PM2.5 sources accounted for 77 % of the total explained variance.  相似文献   

2.
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   

3.
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   

4.
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   

5.
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   

6.
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   

7.
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   

8.
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   

9.
The heterogeneous interaction of nitrogen dioxide with ammonium chloride was investigated in a molecular diffusion tube experiment at 295–335 K and interpreted using Monte Carlo trajectory calculations. The surface residence time (τsurf) of NO2 on NH4Cl is equal to 15 μs at 295 K, increases with temperature up to 323 K (τsurf = 45 μs) and probably decreases beyond 323 K. The same experiment also yields uptake coefficients, γ, which are derived from the absolute number of surviving molecules effusing out of the diffusion tube. The rate of uptake of NO2 on NH4Cl followed a rate law first order in [NO2] and the uptake coefficient γ is equal to 7 × 10−5 at 295 K, increases with temperature up to 323 K (γ = 2.1 × 10−4) and probably decreases beyond 323 K. Nitrous acid, water and nitrogen were detected as products. From these products, it is concluded that the reaction of NO2 with NH4Cl is a reverse disproportionation reaction where two moles of NO2 result in ammonium nitrite, NH4NO2, as an intermediate, and nitryl chloride, NO2Cl. NH4NO2 decomposes in two pathways, one to nitrous acid, HONO and NH3, the other to nitrogen and water. The branching ratio for the production of HONO + NH3 to that of N2 + H2O is approximately 20 at 298 K and increases with increasing temperature.  相似文献   

10.
Factors Influencing Nitrogen Speciation in Coastal Rainwater   总被引：1，自引：0，他引：1  
Rainwater was collected from 129 rain events between February 2002 and August 2003 and analyzed for ammonium (NH4+), nitrate (NO3−), organic nitrogen (ON) and free amino acids (AA). Inorganic nitrogen (NO3− + NH4+) was the dominant form of N representing 85% of total nitrogen based on volume-weighted averages. The remainder of the N occurred as organic nitrogen species of which free amino acids contribute approximately 17%. A significant, and in some cases the majority (> 75%), of the remaining ON could be accounted for by macromolecular uncharacterized humic like substances. This has important ramifications with respect to the long range transport of atmospheric ON because humic materials are recalcitrant and therefore may travel long distances from their source. There was a distinct seasonality to the N speciation data with maximum concentrations of NH4+, ON and AA occurring in the spring. Air-mass back trajectory analysis indicates there is a strong anthropogenic component to the NO3−, NH4+ and AA signal but not ON. There was a strong positive correlation between amino acid concentrations and ammonium which suggests they have similar sources and sinks in rainwater. Finally, large episodic additions of NH4+ and AA during tropical events could significantly impact short term bioavailable N budgets in estuaries impacted by these storms. Approximately three times as much NH4+ and AA were deposited during Hurricane Isabel (317 μ moles ⋅ m−2 and 84 μ moles ⋅ m−2 respectively) compared to the mean impact of average summertime rain events at this location.  相似文献   

11.
Both aerosol and rainwater samples were collected and analyzed for ionic species at a coastal site in Southeast Asia over a period of 9 months (January–September 2006) covering different monsoons. In general, the occurrence and distribution of ionic species showed a distinct seasonal variation in response to changes in air mass origins. Real-time physical characterization of aerosol particles during rain events showed changes in particle number distributions which were used to assess particle removal processes associated with precipitation, or scavenging. The mean scavenging coefficients for particles in the range 10–500 nm and 500–10 μm were 7.0 × 10−5 ± 2.8 × 10−5 s−1 and 1.9 × 10−4 ± 1.6 × 10−5 s−1, respectively. A critical analysis of the scavenging coefficients obtained from this study suggested that the wet removal of aerosol particles was greatly influenced by rain intensity, and was particle size-dependent as well. The scavenging ratios, another parameter used to characterize particle removal processes by precipitation, for NH4 +, Cl−, SO4 2−, and NO3 − were found to be higher than those of Na+, K+, and Ca2+ of oceanic and crustal origins. This enrichment implied that gaseous species NH3, HCl, and HNO3 could also be washed out readily. These additional sources of ions in precipitation presumably counter-balanced the dilution effect caused by high total precipitation volume in the marine and tropical area.  相似文献   

12.
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   

13.
This study systematically analyzed the concentrations of cations and anions and determined the pH in the rainwater at Guiyang from Oct. 2008 to Sep. 2009. The pH in the rainwater varied between 3.35 and 9.99 with a volume-weighted mean value of 4.23. The volume-weighted mean concentrations of anions followed the order SO4 2->Cl->F->NO3 -, whereas the volume-weighted mean concentrations of cations followed the order Ca2+>NH4 +>Na+>Mg2+>K+. This finding indicates that SO4 2- was the main anion and that Ca2+ and NH4 + were the main cations. Significant correlations between each pair of ions (SO4 2-, NO3 -, NH4 +, Ca2+, and Mg2+) were observed, suggesting that CaSO4, Ca(NO3)2, MgSO4, Mg(NO3)2, NH4NO3, (NH4)2SO4, and/or NH4HSO4 exist in the atmosphere at Guiyang. The soil-derived species (such as Ca2+) played an important role in the neutralization of the acidity in rainwater. The SO4 2- and NO3 - in the rainwater were mainly from anthropogenic sources, and their contributions accounted for 98.1 % and 94.7 %, respectively. NH4 + was also most likely derived from anthropogenic sources, such as domestic and commercial sewage, and played an important role in the neutralization of the rainwater at Guiyang.  相似文献   

14.
Simultaneous measurements on physical, chemical and optical properties of aerosols over a tropical semi-arid location, Agra in north India, were undertaken during December 2004. The average concentration of total suspended particulates (TSP) increased by about 1.4 times during intense foggy/hazy days. Concentrations of SO4 2−, NO3 −, NH4 + and Black Carbon (BC) aerosols increased by 4, 2, 3.5 and 1.7 times, respectively during that period. Aerosols were acidic during intense foggy/hazy days but the fog water showed alkaline nature, mainly due to the neutralizing capacity of NH4 aerosols. Trajectory analyses showed that air masses were predominantly from NW direction, which might be responsible for transport of BC from distant and surrounding local sources. Diurnal variation of BC on all days showed a morning and an evening peak that were related to domestic cooking and vehicular emissions, apart from boundary layer changes. OPAC (Optical properties of aerosols and clouds) model was used to compute the optical properties of aerosols. Both OPAC-derived and observed aerosol optical depth (AOD) values showed spectral variation with high loadings in the short wavelengths (<1 μm). AOD value at 0.5 μm wavelength was significantly high during intense foggy/hazy days (1.22) than during clear sky or less foggy/hazy days (0.63). OPAC-derived Single scattering albedo (SSA) was 0.84 during the observational period, indicating significant contribution of absorbing aerosols. However, the BC mass fraction to TSP increased by only 1% during intense foggy/hazy days and thereby did not show any impact on SSA during that period. A large increase was observed in the shortwave (SW) atmospheric (ATM) forcing during intense foggy/hazy days (+75.8 W/m2) than that during clear sky or less foggy/hazy days (+38 W/m2), mainly due to increase in absorbing aerosols. Whereas SW forcing at surface (SUF) increased from −40 W/m2 during clear sky or less foggy/hazy days to −76 W/m2 during intense foggy/hazy days, mainly due to the scattering aerosols like SO4 2-.  相似文献   

15.
Cloud/fog water samples were collected at Daekwanreung (840 m msl), a ridge site, in South Korea, from March 2002 to September 2003, by using a Caltech type, self fabricated active strand cloud water collector. The pH, electrical conductivity and major ion concentrations were analyzed. The cloud water pH ranged from 3.6 to 6.8 with an average of 5.2, which was close to the atmospheric neutral point. However, the pH calculated from average concentrations of H+ was 4.7, indicating the cloud/fog water was weakly acidified. SO4 2−, NO3 − and NH4 + are predominant ions of which average concentrations were 203.1, 128.1, and 211.7 μeq⋅L−1, respectively. Samples were categorized into four groups by applying 48-hour back trajectory analysis, using the HYbrid Single-Particle Largrangian Integrated Trajectory (HYSPLIT) model. Chemical compositions for the four cases significantly differed from each other. For air masses transported from the East Sea (group E), sea salt concentrations, including Na+, Cl− Mg2+, were relatively high. Principal acidifying pollutants, such as NO3 − and nss-SO4 2−, significantly increased in the case of air masses transported from the Northeast Asian continent through North Korea (group N) and air masses from the Seoul metropolitan area (group W). However, the mean pH of group N was the highest while the mean pH of group W was the lowest. This suggests that most NO3 − and nss-SO4 2− in cloud/fog water was neutralized by ammonia and calcium compounds under the influence of air masses transported from Northeast Asia. N/S ratio for the group W was significantly higher than those for the other three groups, suggesting nitrogen species transported from the Seoul metropolitan area contributed to acidification of cloud/fog water at Daekwanreung. Principle Component analysis (PCA) was applied to the cloud/fog water data for presenting characteristics in the four different categories.  相似文献   

16.
Hoarfrost and rime analysis was based on the collection of samples between 2003 and 2006 from 8 sites, which represent both lowland (northern) and mountainous (southern) parts of Poland. On the other hand 4 of these sites belong to “urban” and 4 to “rural” category. pH, conductivity, SO42−, NO3−, Cl−, H+, NH4+, Ca2+, Mg2+, Na+, K+ have been determined in order to study the chemistry of hoarfrost and rime. Higher total inorganic ionic content (TIC) in hoarfrost and rime (2.46 meq·l−1 and 1.23 meq·l−1 respectively) was observed when compared with precipitation (0.37 meq·l−1). Large variability of TIC and chemical composition of individual samples were typical at each of the measurement sites depending on emission patterns, atmospheric conditions and local terrain topography. Higher concentrations of both hoarfrost and rime occurred in southern (mountainous) rather than in northern (lowland) part of Poland which can be explained by worse pollutant dispersion conditions in the south. The surprisingly low hoarfrost concentrations in urban coastal stations in the area of the Bay of Gdansk were attributed to the cleaning effect of nocturnal breeze-type circulation, best pronounced in cool part of the year. Due to relatively high pollutant concentration and long duration, hoarfrost and rime are at least significant factors in environmental processes in different ecosystems in Poland.  相似文献   

17.
In the present study, the wet and dry depositions of particulate NO3−, SO42−, Cl− and NH4+ were measured using a wet/dry sampler as a surrogate surface. Gas phase compounds of nitrogen, sulfur and chloride (HNO3, NH3, SO2 and HCl) were measured by an annular denuder system (ADS) equipped with a back up filter for the collection of particles with diameter ≤ 5 μm. Ambient concentrations of NO, NO2 and SO2 were also taken into consideration. Sampling was conducted at an urban site in the center of the city of Thessaloniki, northern Greece. The presence of the aerosol species was examined by cold/warm period and the possible compounds in dry deposits were also considered. Dry deposition fluxes were found to be well correlated with ambient particle concentrations in order to be used for the calculation of particle deposition velocity. Average particulate deposition velocities calculated were 0.36, 0.20, 0.20 and 0.10 cm s− 1 for Cl−, NO3−, SO42− and NH4+, respectively. Total dry deposition fluxes (gas and particles) were estimated at 3.24 kg ha− 1 year− 1 for chloride (HCl + p-Cl), 9.97 kg ha− 1 year− 1 for nitrogen oxidized (NO + NO2 + HNO3 + p-NO3), 5.32 kg ha− 1 year− 1 for nitrogen reduced (NH3 + p-NH4) and 15.77 kg ha− 1 year− 1 for sulfur (SO2 + p-SO4). 70–90% total dry deposition was due to gaseous species deposition. The contribution of dry deposition to the total (wet + dry) was at the level of 60–70% for sulfur and nitrogen (oxidized and reduced), whereas dry chloride deposition contributed 35% to the total. The dry-to-wet deposition ratio of all the studied species was found to be significantly associated with the precipitation amount, with nitrogen species being better and higher correlated. Wet, dry and total depositions measured in Thessaloniki, were compared with other countries of Europe, US and Asia.  相似文献   

18.
An hourly quantification of inorganic water-soluble PM10 ions and corresponding trace gases was performed using the Monitor for AeRosols and Gases in ambient Air (MARGA) at the TROPOS research site in Melpitz, Germany. The data availability amounts to over 80% for the five-year measurement period from 2010 to 2014. Comparisons were performed for the evaluation of the MARGA, resulting in coefficients of determinations (slopes) of 0.91 (0.90) for the measurements against the SO2 gas monitor, 0.84 (0.88), 0.79 (1.39), 0.85 (1.20) for the ACSM NO3 ?, SO4 2? and NH4 + measurements, respectively, and 0.85 (0.65), 0.88 (0.68), 0.91 (0.83), 0.86 (0.82) for the filter measurements of Cl?, NO3 ?, SO4 2? and NH4 +, respectively. A HONO comparison with a batch denuder shows large scatter (R2 = 0.41). The MARGA HNO3 is underestimated compared to a batch and coated denuder with shorter inlets (slopes of 0.16 and 0.08, respectively). Less NH3 was observed in coated denuders for high ambient concentrations. Long-time measurements show clear daily and seasonal variabilities. Potential Source Contribution Function (PSCF) analysis indicates the emission area of particulate ions Cl?, NO3 ?, SO4 2?, NH4 +, K+ and gaseous SO2 to lie in eastern European countries, predominantly in wintertime. Coarse mode sea salt particles are transported from the North Sea to Melpitz. The particles at Melpitz are nearly neutralised with a mean molar ratio of 0.90 for the five-year study. A slight increase of the neutralization ratio over the last three years indicates a stronger decrease of the anthropogenically emitted NO3 ? and SO4 2? compared to NH4 +.  相似文献   

19.

The present study comprehensively reports the simultaneous measurement of wet deposition of total inorganic nitrogen (TIN; which is the sum of the NH4+-N and NO3?-N) at three different sites in Nr emission hotspot of Indo-Gangetic plain (IGP) over a year-long temporal scale from October 2017 to September 2018. At rural Meetli (MTL) site, urban Baraut (BRT) site and industrial Loni (LNI) site, the annual wet deposition of NH4+-N was estimated as 21.87, 19.48 and 7.43 kg N ha?1 yr?1, respectively; the annual wet deposition NO3?-N was estimated as 12.96, 12.17 and 4.44 kg N ha?1 yr?1, respectively; and the annual wet deposition of TIN was estimated as 34.83, 31.64 and 11.87 kg N ha?1 yr?1, respectively. NH4+-N was dominantly contributing species in annual, monsoon and non-monsoon-time wet deposition of TIN at all sites. The spatial gradient (variability) in percent contribution of NH4+ to total annual volume-weighted mean (VWM) concentration of all analyte ions was observed as MTL (43.23%)?>?BRT (37.90%)?>?LNI (30%). On the other hand, the spatial gradient in percent contribution of NO3? to total annual VWM concentration of all analyte ions was observed as MTL (7.45%)?>?BRT (6.89%)?>?LNI (5.32%). The extremely narrow range of NH4+-N/NO3?-N ratios (ranging from 1.60 at BRT site to 1.69 at LNI site) showed the approximately equal relative abundance of oxidized and reduced nitrogen (N) deposition across all sites. Inferences from enrichment factor analysis, principal component analysis and Pearson’s correlation coefficient analysis suggested that across all sites, virtually all NH4+-N and NO3?-N depositions were originated anthropogenically. The annual wet deposition of TIN measured in this study showed?≥?6865%,?≥?6228% and?≥?2274% increment than the natural N deposition rate at MTL, BRT and LNI site, respectively. These empirically measured annual wet depositions of TIN also emanated theoretical transgression of critical N load threshold across all sites therefore signifying probable undermining of long-term elastic stability and resilience of ecosystems against stressor in the study domain.

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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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