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1.
Fine aerosol samples were collected throughout spring, summer, and winter in 2004∼2005 at a major urban traffic junction (BNU) and a suburban location (MY) in Beijing and at a downtown site (SH) in Shanghai, China. Ten of the 16 EPA priority polycyclic aromatic hydrocarbons (PAHs), seven fatty acids, levoglucosan, and cholesterol were identified and quantified. PAHs detected in Beijing and Shanghai were up to one order of magnitude higher than those reported in the developed countries either in urban or suburban areas, while levoglucosan was one order of magnitude lower than that in other countries for no biomass combustion in domestic heating in the mega-cities in China. PAHs showed the same seasonal trend in all sampling sites as the highest in winter and the lowest in summer, while fatty acids no pronounced seasonal variation. A significant fraction of levoglucosan from cooking with higher concentrations in urban than in suburban area contributed to the ambient atmosphere, indicating that the main source of levoglucosan in urban environment would be cooking rather than biomass burning. The relative contributions of coal combustion and vehicle exhaust sources to PAHs in fine aerosols were preliminarily estimated to be 1:2 in Beijing and 1:1 in Shanghai, revealing that the air pollution in these mega-cities in China was mainly the mixing of coal combustion with vehicle exhaust. Cooking was one of the major sources of organic aerosols in both Beijing and Shanghai.  相似文献   

2.
A coupled aerosol–cloud model is essential for investigating the formation of haze and fog and the interaction of aerosols with clouds and precipitation. One of the key tasks of such a model is to produce correct mass and number size distributions of aerosols. In this paper, a parameterization scheme for aerosol size distribution in initial emission, which took into account the measured mass and number size distributions of aerosols, was developed in the GRAPES–CUACE [Global/Regional Assimilation and PrEdiction System–China Meteorological Administration (CMA) Unified Atmospheric Chemistry Environment model]—an online chemical weather forecast system that contains microphysical processes and emission, transport, and chemical conversion of sectional multi-component aerosols. In addition, the competitive mechanism between nucleation and condensation for secondary aerosol formation was improved, and the dry deposition was also modified to be in consistent with the real depositing length.Based on the above improvements, the GRAPES–CUACE simulations were verified against observational data during 1–31 January 2013, when a series of heavy regional haze–fog events occurred in eastern China. The results show that the aerosol number size distribution from the improved experiment was much closer to the observation, whereas in the old experiment the number concentration was higher in the nucleation mode and lower in the accumulation mode. Meanwhile, the errors in aerosol number size distribution as diagnosed by its sectional mass size distribution were also reduced. Moreover, simulations of organic carbon, sulfate, and other aerosol components were improved and the overestimation as well as underestimation of PM2.5 concentration in eastern China was significantly reduced, leading to increased correlation coefficient between simulated and observed PM2.5 by more than 70%. In the remote areas where bad simulation results were produced previously, the correlation coefficient grew from 0.35 to 0.61, and the mean mass concentration went up from 43% to 87.5% of the observed value. Thus, the simulation of particulate matters in these areas has been improved considerably.  相似文献   

3.
2008年北京奥运会期间大气气溶胶物理特征分析   总被引：5，自引：0，他引：5  
应用MODIS卫星的气溶胶产品资料和地面的光学粒子计数器的资料,对比分析了北京地区2006、2007、2008年7～9月的气溶胶光学厚度、细粒子光学厚度、Angstrom指数、气溶胶粒子数浓度谱及体积谱,发现2008年北京奥运会期间(7月20日～9月20日)的气溶胶光学厚度比2006、2007年同期明显降低,气溶胶细模态光学厚度占总光学厚度的比上升,Angstrom指数上升,气溶胶细粒子数浓度没有明显相对变化,而粗粒子数浓度则减少约50%.利用大气标高,将MODIS反演的气溶胶柱的质量浓度转化为地面气溶胶质量浓度.用粒子计数器得到的体积谱,在假定气溶胶粒子密度的情况下,计算出其质量浓度.将这两种方法得到的气溶胶质量浓度与国家环境保护部公布的空气质量指数换算得到的可吸入颗粒物(PM10)质量浓度进行比较.结果表明:北京奥运期间空气质量总体达到了国家二级空气质量标准;与2006、2007年同期相比,2008年气溶胶PM10质量浓度明显下降,而这主要是由气溶胶粗粒子的减少引起的.  相似文献   

4.
《Atmospheric Research》2009,91(2-4):253-263
A high-volume cascade impactor, equipped with a PM10 inlet, was used to collect size-segregated aerosol samples during the summer of 2004 at two Portuguese locations: a coastal-rural area (Moitinhos) and an urban area (Oporto). Concentrations of airborne particulate matter (PM), total carbon (TC), organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC) were determined for the following particle size ranges: < 0.49, 0.49–0.95, 0.95–3.0, and 3.0–10 µm. The total PM mass concentrations at the urban and coastal-rural sites ranged from 22.8 to 79.6 μg m− 3 and 19.9 to 28.2 μg m− 3, respectively, and more than 56% of the total aerosol mass was found in the fractions below 3.0 μm. At both locations the highest concentrations of OC and EC were found in the submicrometer size range. The regional variability for the OC and EC concentrations, with the highest concentrations being found in the urban area, was related to the contribution of local primary sources (mostly traffic emissions). It was also verified an enrichment of the small size particles in WSOC, representing on average 37.3(± 12.4)% and 59.7(± 18.0)% of OC in the very fine aerosol at the coastal-rural and urban areas, respectively. The amount of secondary OC calculated by the minimum OC/EC ratio method indicates that secondary organic aerosol formation was important throughout the study at both sites. The obtained results suggest that long-range transport and favourable summer conditions for photochemical oxidation are key factors determining secondary OC formation in the coastal-rural and urban areas. The ultraviolet absorption properties of the chromophoric constituents of the WSOC fractions were also different among the different particle size ranges and also between the two sampling locations, thus suggesting the strong impact of the diverse emission sources into the composition of the size-segregated organic aerosol.  相似文献   

5.
A high-volume cascade impactor, equipped with a PM10 inlet, was used to collect size-segregated aerosol samples during the summer of 2004 at two Portuguese locations: a coastal-rural area (Moitinhos) and an urban area (Oporto). Concentrations of airborne particulate matter (PM), total carbon (TC), organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC) were determined for the following particle size ranges: < 0.49, 0.49–0.95, 0.95–3.0, and 3.0–10 µm. The total PM mass concentrations at the urban and coastal-rural sites ranged from 22.8 to 79.6 μg m− 3 and 19.9 to 28.2 μg m− 3, respectively, and more than 56% of the total aerosol mass was found in the fractions below 3.0 μm. At both locations the highest concentrations of OC and EC were found in the submicrometer size range. The regional variability for the OC and EC concentrations, with the highest concentrations being found in the urban area, was related to the contribution of local primary sources (mostly traffic emissions). It was also verified an enrichment of the small size particles in WSOC, representing on average 37.3(± 12.4)% and 59.7(± 18.0)% of OC in the very fine aerosol at the coastal-rural and urban areas, respectively. The amount of secondary OC calculated by the minimum OC/EC ratio method indicates that secondary organic aerosol formation was important throughout the study at both sites. The obtained results suggest that long-range transport and favourable summer conditions for photochemical oxidation are key factors determining secondary OC formation in the coastal-rural and urban areas. The ultraviolet absorption properties of the chromophoric constituents of the WSOC fractions were also different among the different particle size ranges and also between the two sampling locations, thus suggesting the strong impact of the diverse emission sources into the composition of the size-segregated organic aerosol.  相似文献   

6.
This study investigated the optical properties of aerosols involved in different meteorological events, including smog and Asian dust days. Carbonaceous components and inorganic species were measured in Seoul, Korea between 25 and 31 March 2012. Based on the measurements, the optical properties of aerosols were calculated by considering composition, size distribution, and mixing state of aerosols. To represent polydisperse size distributions of aerosols, a lognormal size distribution with a wide range of geometric mean diameters and geometric standard deviations was used. For the optical property calculations, the Mie theory was used to compute single-scattering properties of aerosol particles with varying size and composition. Analysis of the sampled data showed that the water-soluble components of organic matter increased on smog days, whereas crustal elements increased on dust days. The water content significantly influenced the optical properties of aerosols during the smog days as a result of high relative humidity and an increase in the water-soluble component. The absorption coefficients depended on the aerosol mixture type and the aerosol size distributions. Therefore, to improve our knowledge on radiative impacts of aerosols, especially the regional impacts of aerosols in East Asia, accurate measurements of aerosols, such as size distribution, composition, and mixture type, under different meteorological conditions are required.  相似文献   

7.
Size-segregated aerosol samples were collected with a low-pressure impactor (LPI) at urban, roadside and rural sites in winter in Beijing. The size distribution of Polycyclic Aromatic Hydrocarbons (PAHs), organic carbon (OC) and elemental carbon (EC) were measured and this study focused on their size distributions and relationships of PAH to OC/EC. All PAHs show uni-modal at the accumulation mode (0.1–1.8 μm) and almost all PAHs are associated with fine particles. The absence of PAHs in the nucleus mode contributes to the coagulation under the condition of high concentration of the accumulation mode particles. The absence of PAHs in the coarse mode was probably attributed to the low temperature that restrained the redistribution of PAHs from the accumulation mode to the coarse mode. Flu(fluoranthene) and Pyr(pyrene, 4-ring) were the most abundant particulate PAHs ; however, IcdP(indeno[1,2,3-cd]pyrene) and BghiP(benzo[ghi]perylene, 6-ring) were rather low. Diagnostic ratios show vehicle and coal burning were the major sources of PAHs in winter. Ratios at rural site are obviously different from those found at roadside and urban sites. Lower value of OC/EC in the rural area than that in the urban area was probably resulted from coal burning prevailed in the rural area. OC1 and OC2 exhibit uni-mode distribution similar to their particle surface area distribution indicating their existence on particles by adsorption. OC3 and OC4 show bi-mode distribution. Grinding of biomass debris can be a probable source of OC3 and OC4 in the coarse mode. EC1 is mostly from the pyrolysis of OC; however, both the natural and anthropogenic emissions contribute to EC2. The correlation between size-segregated PAHs and carbonaceous component is also discussed to identify their sources.  相似文献   

8.
The indoor PM2.5 aerosol samples for charcoal broiling source under Chinese traditional charbroiling and the ambient fine aerosols samples (PM2.5) were collected in Beijing to investigate the characteristics of the charcoal broiling source and its impact on the fine organic aerosols in the atmosphere. The concentrations of 20 species of the trace organic compounds, including polycyclic aromatic hydrocarbons (PAHs), fatty acids, levoglucosan, and cholesterol in PM2.5 were identified and quantified by GC/MS. The total PAHs and fatty acids emitted from charcoal broiling to PM2.5 were 8.97 and 87,000 ng mg−1 respectively. The concentrations of the light molecular weight (LMW) 3- and 4-ring PAHs were much higher than those of the high molecular weight (HMW) 5- and 6-ring PAHs. Fatty acids were the most abundant species in source profile, accounting for over 90% of all identified organic compounds. More polyunsaturated fatty acid (linoleic acids) than the saturated fatty acid (stearic acids) emitted in the cooking. Charcoal broiling is a minor source of PAHs compared to the source of biomass burning. Comparing the ratios of levoglucosan/fatty acid and levoglucosan/cholesterol in the charcoal broiling samples to the ambient samples, it is evident that meat cooking is an important source of fatty acids, but a less important source of cholesterol. Cooking, as one of the source of fine organic particles, plus other anthropogenic sources would be related to the formation of the severe haze occurred and spread over the urban atmosphere in most of the cities of China in the past several years.  相似文献   

9.
Organic aerosol formation resulting from the ozonolysis of α-pinene, myrcene and sabinene was investigated in a large aerosol chamber in the presence of aqueous seed aerosols. The chemical composition of the particles was monitored by an aerosol mass spectrometer (Aerodyne Research Inc.) as a function of time and the particle size. Smaller particles were found to contain more organics relative to sulfate than the larger ones. In contrast, the water to sulfate mass ratio was not dependent on the particle size. These experimental findings indicate the formation of organic layers on the particles. With the aid of an aerosol dynamic model we demonstrate that the observations are consistent with the formation of multilayered organic films having thicknesses of approximately 10 nm. The results also suggest that the films were formed through condensation of low-volatile oxidation products that did not take up water considerably. Even though dissolution of oxidation products into the particle aqueous phase cannot be conclusively ruled out, the most plausible interpretation of the results is that the monoterpene ozonolysis lead to the formation of organic coatings on aqueous aerosols. Such films are likely to form in regions with monoterpene emissions.  相似文献   

10.
The change of the chemical composition of the near-ground level atmospheric aerosol was studied during two summer episodes by a Lagrangian type of experimental approach. Bulk and single-particle chemical analyses of ions and elements in the particulate phase were deployed. N(-III) and N(V) components were also measured in the gas-phase. The measurements were completed by particle size distributions.Secondary inorganic aerosols (SIA) and fine particles of ≈0.2–0.4 μm size were still elevated 50 km downwind of the city. The direct comparison of transport over the city in contrast to transport over the surrounding areas showed that SIA was formed from emission from the city within less than 3 h. Relative increases, i.e., enrichment during transport were observed for primary and secondary aerosol components. The degree of mixing on the individual particle level increased significantly during transport in the area. In particular, newly emitted carbonaceous particles became internally mixed within hours with pre-existing sulphate particles. Mostly due to secondary aerosol formation the average particle size (mass median diameter) of major constituents of the aerosol was significantly decreased while being transported over 13 h. Given recent insights which link fine particles number and mass concentrations with health risks, the results suggest that rural populations in areas which frequently are located within an urban plume might run an elevated health risk relative to populations in areas not affected by urban plumes.  相似文献   

11.
Characterization of aerosols is required to reduce uncertainties in satellite retrievals of global aerosols and for modeling the effects of these aerosols on climate.Aerosols in the North China Plain(NCP) are complex,which provides a good opportunity to study key aerosol optical properties for various aerosol types.A cluster analysis of key optical properties obtained from Aerosol Robotic Network(AERONET) data in Beijing and Xianghe during 2001-11 was performed to identify dominant aerosol types and their associated optical properties.Five dominant aerosol types were identified.The results show that the urban/industrial aerosol of moderate absorption was dominant in the region and that this type varied little with season.Urban/industrial aerosol of weak absorption was the next most common type and mainly occurs in summer,followed by that strong aerosols occurring mainly in winter.All were predominantly fine mode particles.Mineral dust(MD) and polluted dust(PD) occurred mainly in spring,followed by winter,and their absorption decreased with wavelength.In addition,aerosol dynamics and optical parameters such as refractive index and asymmetry factor were examined.Results show that the size of coarse mode particles decreased with AOD indicating the domination of external mixing between aerosols.  相似文献   

12.
The non-polar organic composition of airborne particulate matter was analysed over a two year period in an urban area under oceanic climate conditions (Errenteria, Basque Country, Spain). In addition, the distribution of polycyclic aromatic hydrocarbons (PAH) among different aerosol particle sizes was determined. Clues as to the origin of various particle types were gained by using scanning electron microscopy to view the morphology of the particulates in each size fraction. Samples were collected on glass fibre filters and analysed by means of soxhlet extraction and gas chromatography (either with a flame ionization detector or coupled to a mass spectrometry). In general, total PAH levels were moderate (0.96–50 ng m− 3) as compared to other studies conducted in Europe, and showed clear seasonal variation with maxima in winter and minima in summer. Vehicular traffic was identified as a major source of PAHs in the study area. Regarding particle size, a bimodal distribution was observed. The large sized particles exhibited an apparent seasonal variation with higher concentrations in winter than in summer. The dependences between particle size, PAH distribution and meteorological variables were studied with multivariate statistics. Three main sources of organic compounds were identified: combustion, vegetation, and atmospheric oxidation.  相似文献   

13.
利用耦合化学过程的区域气候模式RegCM3,模拟研究3种主要人为排放气溶胶(硫酸盐、黑碳、有机碳)对东亚区域气候的影响.计算分析近20 a来3种气溶胶的时空分布、综合辐射强迫作用及其对地面气温和降水的影响.模拟结果表明:3种气溶胶冬夏季分布有所不同,冬季气溶胶大值区主要分布在南方地区,而夏季大值区北移;气溶胶短波辐射强迫在大气层顶和地面均为负值;气溶胶的加入对东亚地区地表气温有明显影响,冬季降温中心位于四川盆地,夏季降温大值区位于华北地区.气溶胶直接气候效应使得冬季东亚大部分地区降水减少,夏季东亚地区降水与中国南方地区夏季气溶胶浓度有较好的相关关系,中国东部雨带有南移趋势.  相似文献   

14.
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15.
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16.
2007年,Ashok等揭示了赤道太平洋区域存在一种三极型分布海表温度异常并称之为厄尔尼诺-Modoki,同时定义了相应的海表温度异常指数EMI（记为IEM）。在此基础上,利用英国哈得来中心逐月海表温度资料、美国NCEP/NCAR月平均再分析数据集、美国国家海洋和大气管理局（NOAA）逐月降水资料（CMAP）,通过在太平洋海表温度异常中扣除厄尔尼诺-Modoki信号后,在Nino1+2区域上定义了东太平洋型海表温度异常指数EPNI（IEPN）。据此,由IEPN和IEM可构成描述热带太平洋海表温度异常变化的一对指数。分析了两个指数相应的海气状态及对海洋性大陆区域气候异常的影响。结果表明,厄尔尼诺-Modoki和东太平洋型海表温度异常及其影响存在显著差异。在北半球夏季,当IEM处于正位相时,热带太平洋海表温度异常呈现“负-正-负”的结构,海洋性大陆大部分区域海表温度异常为负,此时对流层低层太平洋地区辐合,海洋性大陆地区辐散,对流层高层太平洋地区辐散,海洋性大陆地区辐合。对应于辐合辐散中心,存在着自赤道中太平洋分别向赤道东太平洋和海洋性大陆中东部地区的异常垂直环流圈,同时也存在自海洋性大陆西部向印度洋西部的垂直环流。大气在海洋性大陆区域北部加热,南部冷却;在太平洋地区西部加热而东部冷却;在海洋性大陆区域10°N以南降水偏少,而10°N以北降水偏多。当IEPN处于正位相时,热带太平洋海表温度异常呈现“西负东正”分布型,海洋性大陆区域海表温度异常呈现“西正东负”分布,对流层低层海洋性大陆地区辐散中心范围偏大、位置偏东、强度偏强,太平洋地区辐合中心范围偏小、位置偏东,热带环流异常在垂直方向上呈斜压结构,海洋性大陆区域北部大气加热而南部冷却,太平洋地区大气均呈加热正异常,海洋性大陆大部分区域降水均偏少,赤道太平洋降水偏多。以上这些结果有利于深刻理解热带太平洋海表温度异常的特征及其对海洋性大陆区域气候的影响。  相似文献   

17.
(NH4)2SO4, CaCl2, Na2SiO3 and NaNO3 were selected as surrogates of inorganic seed aerosols of ambient atmosphere of Chinese urban areas, respectively, to study their effects on the formation of secondary organic aerosol (SOA) in the toluene/CH3ONO/NOx photooxidation system. The SMPS and aerosol laser time-of-flight mass spectrometer (ALTOFMS) was used to measure the aerodynamic size and chemical composition of individual SOA particles in real-time. Experimental results indicate that either the growth or products of SOA is affected by the presence of inorganic seed aerosol. Inorganic seed aerosols would promote growth rates of SOA formation at the start of the reaction and inhibits its formation rate with prolonging the reaction time. In the case of about 100 μg m?3 seed aerosol load, the addition of Na2SiO3 induced a same growth rate of SOA formation as NaNO3. The influence of four individual seed aerosols on the generation of SOA decreased in the order of CaCl2 > (NH4)2SO4 > NaNO3, Na2SiO3. The presence of Na2SiO3 or NaNO3 has no obvious effect on the growth rates of SOA formation, but it does increase the yield of organic acid and nitrogen-containing organic compounds, respectively. Besides the significantly effect on the growth rate of SOA formation, the presence of CaCl2 or (NH4)2SO4 can lead to the formation of high-molecular weight species which is found to be positively correlated with the hygroscopic behavior of seed aerosols. The CaCl2 shows the strongest hygroscopic behavior among the four individual seed aerosols, and the most significant promotion effect on the formation of the high-molecular weight species. It is proposed that the SOA generation enhancement and high-molecular weight products are achieved by particle-phase heterogeneous reactions induced and catalyzed by the acidity of CaCl2 and (NH4)2SO4 seed aerosols.  相似文献   

18.
Surface measurements of aerosol physical properties were made at Anantapur(14.62°N,77.65 °E,331 m a.s.l),a semiarid rural site in India,during August 2008-July 2009.Measurements included the segregated sizes of aerosolsas as well as total mass concentration and size distributions of aerosols measured at low relative humidity(RH<75%) using a Quartz Crystal Microbalance(QCM) in the 25-0.05 μm aerodynamic diameter range.The hourly average total surface aerosol mass concentration in a day varied from 15 to 70 μg m-3,with a mean value of 34.02±9.05μgm-3 for the entire study period.A clear diurnal pattern appeared in coarse,accumulation and nucleation-mode particle concentrations,with two local maxima occurring in early morning and late evening hours.The concentration of coarse-mode particles was high during the summer season,with a maximum concentration of 11.81±0.98μgm-3 in the month of April,whereas accumulationmode concentration was observed to be high in the winter period contributed >68% to the total aerosol mass concentration.Accumulation aerosol mass fraction,A f(=Ma/Mt) was highest during winter(mean value of Af～0.80) and lowest(Af～0.64) during the monsoon season.The regression analysis shows that both R eff and R m are dependent on coarse-mode aerosols.The relationship between the simultaneous measurements of daily mean aerosol optical depth at 500 nm(AOD500) and PM 2.5 mass concentration([PM2.5]) shows that surface-level aerosol mass concentration increases with the increase in columnar aerosol optical depth over the observation period.  相似文献   

19.
上海市区和郊区黑碳气溶胶的观测对比   总被引：11，自引：0，他引：11       下载免费PDF全文
为了探讨上海市区和郊区黑碳气溶胶质量浓度、分布以及来源和输送等特征,利用上海浦东 (市区) 和东滩 (郊区河口湿地)2007年12月—2008年11月的黑碳气溶胶小时平均质量浓度数据,对比分析了两地黑碳气溶胶浓度在不同时间尺度上的变化特征以及气象要素对黑碳质量浓度的影响。结果表明:观测期间浦东和东滩两地黑碳气溶胶小时质量浓度平均值分别为3.8 μg·m-3,1.7 μg·m-3。两地黑碳气溶胶浓度具有类似的季节变化特征,均为冬季较高、夏季较低;同时浦东黑碳气溶胶浓度日变化呈现出明显的双峰结构,并具有显著的周末效应,体现了局地人为源排放的影响。受源排放影响为主的市区与受输送影响为主的郊区,黑碳气溶胶浓度在不同风向上与风速的关系表现出不同特征。  相似文献   

20.
Outdoor smog chamber experiments were performed to investigate gas/particle (G/P) partitioning behavior of aldehyde compounds in atmospheric acidic aerosols. Diesel soot and wood smoke aerosols were selected as acidic aerosols and octanal, decanal, undecanal, and cis-pinonaldehyde for aldehydes compounds. Aerosol acidity was measured with the equivalent sulfuric acid amounts in aerosol mass: 0.2–0.6 wt% in diesel soot and 0.04–0.1 wt% in wood smoke aerosols. Experimentally determined partitioning coefficients of aldehyde along with other classes of semivolatile organic compounds (SOCs) were compared with the estimation. All experimental G/P partitioning coefficients of aldehyde compounds were 10–200 times higher than estimated partitioning coefficients. Aldehyde partitioning coefficients in wood soot were similar or less than diesel soot aerosols.  相似文献   

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