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1.
Haze-fog conditions over northern India are associated with visibility degradation and severe attenuation of solar radiation by airborne particles with various chemical compositions. PM2.5 samples have been collected in Delhi, India from December 2011 to November 2012 and analyzed for carbonaceous and inorganic species. PM10 measurements were made simultaneously such that PM10–2.5 could be estimated by difference. This study analyzes the temporal variation of PM2.5 and carbonaceous particles (CP), focusing on identification of the primary and secondary aerosol emissions, estimations of light extinction coefficient (bext) and the contributions by the major PM2.5 chemical components. The annual mean concentrations of PM2.5, organic carbon (OC), elemental carbon (EC) and PM10–2.5 were found to be 153.6 ± 59.8, 33.5 ± 15.9, 6.9 ± 3.9 and 91.1 ± 99.9 μg m?3, respectively. Total CP, secondary organic aerosols and major anions (e.g., SO4 2? and NO3 ?) maximize during the post-monsoon and winter due to fossil fuel combustion and biomass burning. PM10–2.5 is more abundant during the pre-monsoon and post-monsoon. The OC/EC varies from 2.45 to 9.26 (mean of 5.18 ± 1.47), indicating the influence of multiple combustion sources. The bext exhibits highest values (910 ± 280 and 1221 ± 371 Mm?1) in post-monsoon and winter and lowest in monsoon (363 ± 110 and 457 ± 133 Mm?1) as estimated via the original and revised IMPROVE algorithms, respectively. Organic matter (OM =1.6 × OC) accounts for ~39 % and ~48 % of the bext, followed by (NH4)2SO4 (~21 % and ~24 %) and EC (~13 % and ~10 %), according to the original and revised algorithms, respectively. The bext estimates via the two IMPROVE versions are highly correlated (R2 = 0.95, root mean square error = 38 % and mean bias error = 28 %) and are strongly related to visibility impairment (r = ?0.72), mostly associated with anthropogenic rather than natural PM contributions. Therefore, reduction of CP and precursor gas emissions represents an urgent opportunity for air quality improvement across Delhi.  相似文献   

2.
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   

3.
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   

4.
Beijing is one of the largest and most densely populated cities in China. PM2.5 (fine particulates with aerodynamic diameters less than 2.5 μm) pollution has been a serious problem in Beijing in recent years. To study the temporal and spatial variations in the chemical components of PM2.5 and to discuss the formation mechanisms of secondary particles, SO2, NO2, PM2.5, and chemical components of PM2.5 were measured at four sites in Beijing, Dingling (DL), Chegongzhuang (CG), Fangshan (FS), and Yufa (YF), over four seasons from 2012 to 2013. Fifteen chemical components, including organic carbon (OC), elemental carbon (EC), K+, NH4 +, NO3 ?, SO4 2?, Cl?, Al, Ca, Fe, Mg, Na, Pb, Si, and Zn, were selected for analysis. Overall, OC, SO4 2?, NO3 ?, and NH4 + were dominant among 15 components, the annual average concentrations of which were 22.62 ± 21.86, 19.39 ± 21.06, 18.89 ± 19.82, and 13.20 ± 12.80 μg·m?3, respectively. Compared with previous studies, the concentrations of NH4 + were significantly higher in this study. In winter, the average concentrations of OC and EC were, respectively, 3 and 2.5 times higher than in summer, a result of coal combustion during winter. The average OC/EC ratios over the four sites were 4.9, 7.0, 8.1, and 8.4 in spring, summer, autumn, and winter, respectively. The annual average [NO3 ?]/[SO4 2?] ratios in DL, CG, FS, and YF were 1.01, 1.25, 1.08, and 1.12, respectively, which were significantly higher than previous studies in Beijing, indicating that the contribution ratio of mobile source increased in recent years in Beijing. Analysis of correlations between temperature and relative humidity and between SOR ([SO4 2?]/([SO4 2?] + [SO2])) and NOR ([NO3 ?]/([NO3 ?] + [NO2])) indicated that gas-phase oxidation reactions were the major formation mechanism of SO4 2? in spring and summer in urban Beijing, whereas slow gas-phase oxidation reactions and heterogeneous reactions both occurred in autumn and winter. NO3 ? was mainly formed through year-round heterogeneous reactions in urban Beijing.  相似文献   

5.
Aerosol size distributions were measured with Micro Orifice Uniform Deposit Impactor (MOUDI) cascade impactors at the rural Angiola and urban Fresno Supersites in California's San Joaquin Valley during the California Regional PM10/PM2.5 Air Quality Study (CRPAQS) winter campaign from December 15, 2000 to February 3, 2001. PM2.5 filter samples were collected concurrently at both sites with Sequential Filter Samplers (SFS). MOUDI nitrate (NO3) concentrations reached 66 μg/m3 on January 6, 2001 during the 1000–1600 PST (GMT-8) period. Pair-wise comparisons between PM2.5 MOUDI and SFS concentrations revealed high correlations at the Angiola site (r > 0.93) but more variability (r < 0.85) at the Fresno site for NO3, sulfate (SO4=), and ammonium (NH4+). Correlations were higher at Fresno (r > 0.87) than at Angiola (r < 0.7) for organic carbon (OC), elemental carbon (EC), and total carbon (TC). NO3 and SO4= size distributions in Fresno were multi-modal and wider than the uni-modal distributions observed at Angiola. Geometric mean diameters (GMD) were smaller for OC and EC than for NO3 and SO4= at both sites. OC and EC were more concentrated on the lowest MOUDI stage (0.056 µm) at Angiola than at Fresno. The NO3 GMD increased from 0.97 to 1.02 µm as the NO3 concentration at Angiola increased from 43 to 66 µg m− 3 during a PM2.5 episode from January 4–7, 2001. There was a direct relationship between GMD and NO3 and SO4= concentrations at Angiola but no such relationships for OC or EC. This demonstrates that secondary aerosol formation increases both concentration and particle size for the rural California environment.  相似文献   

6.
Severe air pollution with visibility deterioration has long been a focus in the North China Plain (NCP). In this study, concentration and light extinction analysis of PM2.5 chemical components were carried out from 2014 to 2017 to study the pollution characteristics in Baoding, a case city of the NCP. The annual average concentration of total PM2.5 components showed a declining trend, decreasing by 11 µg m−3 (water-soluble inorganic ions), 23 µg m−3 (carbonaceous aerosols), and 1796 ng m−3 (inorganic elements). Contributing 82.9% to the concentration of total ions, the dominant components, NH4+, NO3, and SO42− became the main pollutants in PM2.5 pollution. Based on the IMPROVE algorithm, the average reconstructed PM2.5 mass concentration was 93 ± 69 µg m−3 during the observation period. Meanwhile, the light extinction coefficients were 373.8 ± 233.6 M m−1, 405.3 ± 300.1 M m−1, 554.3 ± 378.2 M m−1 and 1005.2 ± 750.3 M m−1, in spring, summer, autumn, and winter, respectively. Ammonium sulfate, ammonium nitrate, and organic matter were the largest contributors to light extinction, accounting for a total of 55%–77% in the four seasons. The bsca (light scattering by particles and gases) reconstructed from PM2.5 components (Rbsca) and the bsca converted from visibility (Vbsca) were compared to evaluate the performance of the IMPROVE algorithm, revealing a high correlation coefficient of 0.84. The high values of Vbsca were underestimated while the low values were overestimated, as determined through comparison with the one-to-ne line. Especially, when Rbsca > 1123 M m−1 (corresponding to < 2.0 km, approximately), Vbsca was underestimated by 17.6%. PM2.5 mass concentration and relative humidity also had an impact on the estimation.摘要华北平原大气污染与低能见度状况一直是人们关切的问题.本文通过分析2014 - 2017年PM2.5化学成分的浓度和消光效果, 研究了华北平原典型城市保定市的大气污染特征.结果表明, PM2.5组分的年均浓度显示下降趋势, 水溶性无机离子,碳质气溶胶和金属元素分别减少了11 µg m−3, 23 µg m−3和1796 ng m−3.NH4+,NO3和SO42−是PM2.5污染的主要污染物, 三者之和占总离子浓度的82.9%.基于IMPROVE方程对细颗粒物进行重构, 在观测期间PM2.5质量浓度平均为93 ± 69 µg m−3, 春季,夏季,秋季和冬季的消光系数分别为373.8 ± 233.6 M m−1,405.3 ± 300.1 M m−1,554.3 ± 378.2 M m−1和1005.2 ± 750.3 M m−1.硫酸铵,硝酸铵和有机物对消光的贡献最大, 不同季节下占比达55% ~77%.通过PM2.5组分进行重构, 利用IMPROVE算法计算得到Rbsca, 用能见度测量值转换得到Vbsca, 二者具有较高的相关性 (r2=0.84) ;但存在Vbsca的高值被低估, Vbsca的低值被高估的现象;特别是当Rbsca > 1123 M m−1 (对应能见度约小于2.0 km) 时, Vbsca的值被低估了17.6%.高浓度PM2.5和高湿度对IMPROVE算法结果有显著的影响.  相似文献   

7.
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   

8.
2018年1月,利用颗粒物采样器采集武汉市大气PM2.5样品并进行水溶性无机离子(F-、Cl-、NO3-、SO42-、Na+、NH4+、K+、Mg2+、Ca2+)的分析.结果表明,NO3-、SO42-、NH4+是PM2.5中最主要的3种水溶性无机离子,除Mg2+与Ca2+外,PM2.5与WSⅡs (水溶性无机离子)之间的相关性显著,且移动源贡献占主导地位.阴阳离子平衡表明武汉市冬季灰霾期PM2.5呈中性或弱酸性.通过混合单粒子拉格朗日综合轨迹模式模拟并采用分层聚类得出了4种主要的后向气流轨迹及相应的PM2.5和水溶性离子浓度,结果表明区域传输对此次灰霾期影响较大.  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.
本文利用2014年全年北京市12个空气质量监测站的逐小时PM_(2.5)地面观测资料,以及Terra卫星和Aqua卫星的MODIS 3 km气溶胶光学厚度(AOD)产品,分析了地面PM_(2.5)和两颗卫星AOD的时空分布特征,并在时空匹配的基础上,建立了AOD与PM_(2.5)浓度之间的回归模型。结果表明:PM_(2.5)浓度在城区高、郊区低,最低值位于定陵站,城区站和郊区站的逐时PM_(2.5)浓度的日变化分别呈"双峰型"和"单峰型";两颗卫星AOD数值也均是城区高、郊区低,沿山区的边界有明显的AOD梯度,且城区上午Terra卫星的AOD高于下午Aqua卫星的AOD,而郊区上、下午的AOD基本相同;Aqua卫星AOD与PM_(2.5)的确定系数(R2)较Terra卫星AOD与PM_(2.5)的确定系数平均高0.11,且城区站点两颗卫星AOD与PM_(2.5)相关性均较郊区站点AOD与PM_(2.5)相关性偏高;综合来看,Aqua卫星的AOD与城区的PM_(2.5)相关系数最高,即Aqua卫星的AOD更适于监测和反演城区地面的PM_(2.5)。  相似文献   

11.
Gaseous pollutants and PM2.5 aerosol particles were investigated during a tropical storm and an air pollution episode in southern Taiwan. Field sampling and chemical analysis of particulate matter and gaseous pollutants were conducted in Daliao and Tzouying in the Kaohsiung area, using a denuder-filter pack system during the period of 22 October to 3 November 2004. Sulfate, nitrate and ammonium were the major ionic species in the PM2.5, accounting for 46 and 39% of the PM2.5 for Daliao and Tzouying, respectively. Higher PM2.5, Cl?, NO3? and NH4+, HNO2 and NH3 concentrations were found at night in both stations, whereas higher HNO3 was found during the day. In general, higher PM2.5, HCl, NH3, SO2, Cl?, NO3?, SO42? and NH4+ concentrations were found in Daliao. The synoptic weather during the experiment was first influenced by Typhoon NOCK-TEN, which resulted in the pollutant concentrations decreasing by about two-thirds. After the tropical thunderstorm system passed, the ambient air quality returned to the previous condition in 12 to 24 h. When there was a strong subsidence accompanied by a high-pressure system, a more stable environment with lower wind speed and mixing height resulted in higher PM2.5, as well as HNO2, NH3, SO42?, Cl?, NO3?, NH4+ and K+ concentrations during the episode days. The rainfall is mainly a scavenger of air pollutants in this study, and the stable atmospheric system and the high emission loading are the major reasons for high air pollutant concentrations.  相似文献   

12.
Intensive measurements of gas and aerosol for 2 weeks were carried out at Qingdao (gas and aerosol in 2000, 2001 and 2002), Fenghuangshan (gas and aerosol in 2000 and 2001), and Dalian (aerosol in 2002) in the winter–spring period. High SO2 episodes were observed on 18 January 2000 at both Qingdao and Fenghuangshan. According to back trajectory calculations and analysis of gaseous species, high SO2 episodes were caused by local pollution and transport.Nitrate, sulfate and ammonium were the major species in PM2.5. Mass fractions of NO3, nss-SO42− and NH4+ at Qingdao in 2002 were 10%, 12% and 5.5% for PM2.5, respectively, which were higher than that of nss-Ca2+ (1%). Chemical compositions observed at Dalian and Fenghuangshan were similar to those at Qingdao. The mass ratio of nss-SO42−/SO2 at Qingdao in winter was low (< 1.2), indicating that sulfate was probably produced by the slow oxidation of SO2 in the gas phase and/or was transported from outside of Qingdao in winter. The equivalent ratio of NH4+ to nss-SO42− was 1.39, suggesting that ammonium sulfate was one of the major chemical compositions in PM2.5. The NO3/SO42− ratio at Qingdao was higher than that at remote places in East Asia. Gas and aerosol data obtained at Fenghuangshan were similar to data at Qingdao, suggesting that emissions from small cities may have a great influence on pollution in northern China.  相似文献   

13.
Based on observations of urban mass concentration of fine particulate matter smaller than 2.5 μm in diameter (PM2.5), ground meteorological data, vertical measurements of winds, temperature, and relative humidity (RH), and ECMWF reanalysis data, the major changes in the vertical structures of meteorological factors in the boundary layer (BL) during the heavy aerosol pollution episodes (HPEs) that occurred in winter 2016 in the urban Beijing area were analyzed. The HPEs are divided into two stages: the transport of pollutants under prevailing southerly winds, known as the transport stage (TS), and the PM2.5 explosive growth and pollution accumulation period characterized by a temperature inversion with low winds and high RH in the lower BL, known as the cumulative stage (CS). During the TS, a surface high lies south of Beijing, and pollutants are transported northwards. During the CS, a stable BL forms and is characterized by weak winds, temperature inversion, and moisture accumulation. Stable atmospheric stratification featured with light/calm winds and accumulated moisture (RH > 80%) below 250 m at the beginning of the CS is closely associated with the inversion, which is strengthened by the considerable decrease in near-surface air temperature due to the interaction between aerosols and radiation after the aerosol pollution occurs. A significant increase in the PLAM (Parameter Linking Aerosol Pollution and Meteorological Elements) index is found, which is linearly related to PM mass change. During the first 10 h of the CS, the more stable BL contributes approximately 84% of the explosive growth of PM2.5 mass. Additional accumulated near-surface moisture caused by the ground temperature decrease, weak turbulent diffusion, low BL height, and inhibited vertical mixing of water vapor is conducive to the secondary aerosol formation through chemical reactions, including liquid phase and heterogeneous reactions, which further increases the PM2.5 concentration levels. The contribution of these reaction mechanisms to the explosive growth of PM2.5 mass during the early CS and subsequent pollution accumulation requires further investigation.  相似文献   

14.
To characterize atmospheric particulate matter equal or less than 2.5 μm in diameter (PM2.5) over the Tropical Atlantic Ocean, aerosol sampling was carried out in Puerto Rico during August and September, 2006. Aerosols were analyzed by ion chromatography for water-soluble inorganic and organic ions (including Na+, NH4 +, Mg2+, Ca2+, K+, Cl?, SO4 2?, NH4 +, F?, methanesulfonate (MSA), and oxalate), by inductive coupled plasma mass spectrometry (ICPMS) for trace elements (Al, Fe, Zn, Mn, Cu, Ni, V, Pb, Cr, Sb, Co, Sc, Cd), and by scanning electron microscopy for individual aerosol particle composition and morphology. The results show that the dominant cations in aerosols were Na+, (mean: 631 ng m?3), accounting for 63.8 % of the total cation and NH4 + (mean: 164 ng m?3), accounting for 13.8 % of the total cation measured in this study. The main inorganic anions were Cl? (576 ng m?3, 54.1 %) and SO4 2? (596 ng m?3, 38.0 %). The main organic anion was oxalate (18 ng m?3). Crustal enrichment factor calculations identified 62 % of the trace elements measured (Cu, Ni, V, Co, Al, Mn, Fe, Sc, and Cr) with crustal origin. Single particle analysis demonstrated that 40 % of the aerosol particles examined were Cl? rich particles as sodium chloride from seawater and 34 % of the total particles were Si-rich particles, mainly in the form of aluminosilicates from dust material. Based on the combination of air-mass trajectories, cluster analysis and principal component analysis, the major sources of these PM2.5 particles include marine, Saharan dust and biomass burning from West Africa; however, volcanic emissions from the Soufriere Hills in Montserrat had significant impact on aerosol composition in this region at the time of sample collection.  相似文献   

15.
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   

16.
Ammonia has a short residence time in the atmosphere and rapidly neutralizes acid gases that occur near its source, requiring a rapid measurement system for ammonia and particulate ammonium concentrations to better understand their sources, temporal variation of ammonia emissions, and the formation of secondary ammonium aerosols. A semi-continuous measurement system, consisting of a diffusion scrubber, a particle growth chamber, an air-liquid separator, and a fluorescent detector, was developed to determine both gaseous ammonia (NH3) and particulate ammonium (NH 4 + ) in PM2.5 in the ambient atmosphere of Gwangju, South Korea, during the months of March, April, July, and September of 2007. During the sampling periods, the average concentrations of ammonia and ammonium were found to be 2.33?±?1.29 μg/m3 and 1.89?±?0.99 μg/m3, respectively. Although the average gaseous ammonia concentration was highest in March, the particulate ammonium concentration was higher during the warmer season, reaching 2.08?±?1.07 μg/m3 and 2.32?±?0.94 μg/m3 in April and July, respectively, while only 1.68?±?0.61 μg/m3 in March and 1.24?±?0.99 μg/m3 in September. It is proposed that the higher availability of acid species during the warmer months produced a significant amount of particulate ammonium sulfate. Diurnal fluctuation of ammonia and ammonium during the warmer months showed that their peak time occurred at approximately 10:00 am. Both ammonia and ammonium concentrations were better correlated during the warmer months than during the cooler months. Further, the data suggest that the ammonia and ammonium were measured under well dispersed conditions, and multiple sources contributed to the ammonia at the sampling site.  相似文献   

17.
Particle light absorption (bap), black carbon (BC), and elemental carbon (EC) measurements at the Fresno Supersite during the summer of 2005 were compared to examine the equivalency of current techniques, evaluate filter-based bap correction methods, and determine the EC mass absorption efficiency (σap) and the spectral dependence of bap. The photoacoustic analyzer (PA) was used as a benchmark for in-situ bap. Most bap measurement techniques were well correlated (r ≥ 0.95). Unadjusted Aethalometer (AE) and Particle Soot Absorption Photometer (PSAP) bap were up to seven times higher than PA bap at similar wavelengths because of absorption enhancement by backscattering and multiple scattering. Applying published algorithms to correct for these effects reduced the differences to 24 and 17% for the AE and PSAP, respectively, at 532 nm. The Multi-Angle Absorption Photometer (MAAP), which accounts for backscattering effects, overestimated bap relative to the PA by 51%. BC concentrations determined by the AE, MAAP, and Sunset Laboratory semi-continuous carbon analyzer were also highly correlated (r ≥ 0.93) but differed by up to 57%. EC measured with the IMPROVE/STN thermal/optical protocols, and the French two-step thermal protocol agreed to within 29%. Absorption efficiencies determined from PA bap and EC measured with different analytical protocols averaged 7.9 ± 1.5, 5.4 ± 1.1, and 2.8 ± 0.6 m2/g at 532, 670, and 1047 nm, respectively. The Angström exponent (α) determined from adjusted AE and PA bap ranged from 1.19 to 1.46. The largest values of α occurred during the afternoon hours when the organic fraction of total carbon was highest. Significant biases associated with filter-based measurements of bap, BC, and EC are method-specific. Correcting for these biases must take into account differences in aerosol concentration, composition, and sources.  相似文献   

18.

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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19.
蔡敏  严明良  包云轩 《气象科学》2018,38(5):648-658
为了探明PM_(2.5)中水溶性无机离子的来源和气象因子对其浓度变化的影响,利用2012年2、5、8和11月苏州市PM_(2.5)中水溶性无机离子浓度和本站气象观测数据,分析了苏州市水溶性无机离子的时间变化特征,解析了当地PM_(2.5)中水溶性无机离子的主要来源,探讨了气象因素对离子组分的影响。结果表明:(1)苏州市PM_(2.5)中水溶性无机离子年均浓度大小依次为:SO_4~(2-)NO_3~-NH_4~+Na~+Cl~-K~+Ca~(2+)Mg~(2+)F~-;SO_4~(2-)、NH_4~+和NO_3~-为PM_(2.5)中最重要的3种水溶性无机离子物种,其总和占PM_(2.5)总质量浓度的50.9%。各离子的季节浓度特征均为冬季最高、夏季最低。(2)通过运用主成分分析法对苏州市PM_(2.5)中水溶性无机离子进行来源分类解析,发现第一类为二次污染源和生物质燃烧,其贡献率为32.84;第二类为道路扬尘及工业排放,其贡献率为19.99%;第三类为海盐污染,其贡献率为18.43%。(3)通过水溶性无机离子与气象条件的相关性分析发现,风向、风速和温度与水溶性无机离子浓度的相关性较显著,这三者是颗粒物浓度变化的主要影响因子。(4)利用HYSPLIT后向轨迹模式对外来污染物进入苏州市的轨迹进行聚类分析后发现:因受季风气候影响,苏州市外来污染物的输入路径存在明显的季节性变化特征,其中夏半年输送主径源自海上,冬半年主径源自内陆。  相似文献   

20.
《Atmospheric Research》2007,83(3-4):688-697
Intensive measurements of gas and aerosol for 2 weeks were carried out at Qingdao (gas and aerosol in 2000, 2001 and 2002), Fenghuangshan (gas and aerosol in 2000 and 2001), and Dalian (aerosol in 2002) in the winter–spring period. High SO2 episodes were observed on 18 January 2000 at both Qingdao and Fenghuangshan. According to back trajectory calculations and analysis of gaseous species, high SO2 episodes were caused by local pollution and transport.Nitrate, sulfate and ammonium were the major species in PM2.5. Mass fractions of NO3, nss-SO42− and NH4+ at Qingdao in 2002 were 10%, 12% and 5.5% for PM2.5, respectively, which were higher than that of nss-Ca2+ (1%). Chemical compositions observed at Dalian and Fenghuangshan were similar to those at Qingdao. The mass ratio of nss-SO42−/SO2 at Qingdao in winter was low (< 1.2), indicating that sulfate was probably produced by the slow oxidation of SO2 in the gas phase and/or was transported from outside of Qingdao in winter. The equivalent ratio of NH4+ to nss-SO42− was 1.39, suggesting that ammonium sulfate was one of the major chemical compositions in PM2.5. The NO3/SO42− ratio at Qingdao was higher than that at remote places in East Asia. Gas and aerosol data obtained at Fenghuangshan were similar to data at Qingdao, suggesting that emissions from small cities may have a great influence on pollution in northern China.  相似文献   

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