Continuous Measurement of Number Concentrations and Elemental Composition of Aerosol Particles for a Dust Storm Event in Beijing

A continuous measurement of number size distributions and chemical composition of aerosol particles was conducted in Beijing in a dust storm event during 21-26 March 2001. The number concentration of coarse particles （ 〉2μm） increased more significantly than fine particles （ 〈2μm） during the dust storm due to dust weather, while the anthropogenic aerosols collected during the non-dust-storm period tended to be associated with fine particles. Elemental compositions were analyzed by using proton-induced X-ray emission （PIXE）. The results show that 20 elements in the dust storm were much higher than in the non-dust-storm period. The calculated soil dust concentration during the dust storm was, on average, 251.8μg m^-3, while it was only 52.1μg m^-3 on non-dust-storm days. The enrichment factors for Mg, A1, P, K, Ca, Ti, Mn, Fe, C1, Cu, Pb, and Zn show small variations between the dust storm and the non-dust-storm period, while those for Ca, Ni and Cr in the dust storm were much lower than those in the non-dust-storm period due to significant local emission sources. A high concentration and enrichment factor for S were observed during the dust storm, which implies that the dust particles were contaminated by aerosol particles from anthropogenic emissions during the long-range transport. A statistical analysis shows that the elemental composition of particles collected during the dust storm in Beijing were better correlated with those of desert soil colleted from desert regions in Inner Mongolia. Air mass back-trajectory analysis further confirmed that this dust storm event could be identified as streaks of dust plumes originating from Inner Mongolia.     

METEOROLOGICAL AND CHEMICAL CONTROLS ON THE VERTICAL DISTRIBUTION OF BEIJING SUMMER COARSE AND FINE AEROSOLS

Vertical profiles of fine and coarse aerosol particles were determined by cascade impaetors at the meteorological tower in Beijing for three days and one night, July 18-23, 1980. Coarse mode aerosols showed a maximum concentration at 47 m when there was an inversion at about 140 m height, and a rather uniform distribution when there was no inversion. This may indicate a two-component origin of coarse particles at the tower site, one being surface dust and the other being tall stack emissions. Fine mode aerosols showed more complex vertical profiles. Median particle size distributions of most metals were bimodat, indicating distinct coarse particle dispersion and fine accumulation mode processes. A chemical thermodynamfc calculation indicates that fine mode Si can result from the reduction of silica to volatile SiO during coal combustion with limited air supply, a process which should release substantial amounts of carbon monoxide to the atmosphere.     

Identification of Aerosol Types and Their Optical Properties in the North China Plain Based on Long-Term AERONET Data

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.     

Characteristics of Aerosol Ionic Compositions in Summer 2003 at Lin''''an of Yangtze Delta Region

With the size-resolved aerosol mass and ion composition data obtained at Lin'an regional atmospheric pollution monitoring station in July 2003, the size distributions of aerosol mass and ionic components, and the correlations between major ion pairs were analyzed. The primary results indicate that in the period of in-situ measurement, the aerosols are mainly composed of fine particles. The mass of aerosols with size less than 2.1μm accounts for 66% of the total mass of all size ranges, in which about 50% of the mass is contributed by the particles with size less than 0.65μm. Similar to the size distributions of aerosol mass, the water-soluble ions are mainly concentrated in the size range of <0.65μm, accounting for about 77% of the sum of analyzed ions, and the ions within the range of <2.1μm reach 88%. The sulfate, ammonium, and potassium are the dominant ionic components in fine particles (particle size less than 2.1μm). Ion correlation analysis suggests that the sulfates in fine particles are mostly in the compounds of (NH4)2SO4, Na2SO4, and K2SO4, but for submicron particles the sulfates are mainly in the form of (NH4)2SO4.     

Temporal Variability in Fine Carbonaceous Aerosol over Two Years in Two Megacities： Beijing and Toronto

Time-series of weekly total carbon(TC)concentrations of fine aerosol particles(PM2.5)in Beijing and Toronto were compared to investigate their respective levels and temporal patterns over two years from August 2001 through July 2003.In addition to this comparison,differences in the factors contributing to the observed concentrations and their temporal variations are discussed.Based upon past knowledge about the two megacities with highly contrasting air pollutant levels,it is not surprising that the average TC concentration in Beijing(31.5μg C m-3)was greater than that in Toronto by a factor of 8.3.Despite their large concentration differences,in both cities TC comprised a similarly large component of PM2.5.TC concentrations exhibited very different seasonal patterns between the two cities.In Beijing,TC experienced higher levels and greater weekly fluctuations in winter whereas in Toronto this behavior was seen in summer. As a result,the greatest gap in TC concentrations between Beijing and Toronto(by a factor of 12.7) occurred in winter,while the smallest gap(a factor of 4.6)was in summer.In Beijing,seasonal variations in the emissions probably played a greater role than meteorology in influencing the TC seasonality,while in Toronto during the warm months more than 80%of the hourly winds were recorded from the south,along with many potential anthropogenic sources for the days with high TC concentrations.This comparison of the differences provides insight into the major factors affecting carbonaceous aerosol in each city.     

AN ANALYSIS OF THE AEROSOLS IN THE LOWER-LEVEL ATMOSPHERE OVER BEIJING NORTHERN SUBURBS IN WINTER*

The physical and chemical characteristics of the aerosol samples were studied.The samples were collected on the 3 platforms (at levels 8 m,100 m and 320 m respectively) of IAP (Institute of Atmospheric Physics,Chinese Academy of Sciences) observation tower during the periods from January 1 to 16 and from February 20 to March 2,2001.The concentrations of TSP (total suspended particles),chemical components and size distribution for aerosols were calculated.The effects of the meteorological conditions on the aerosol concentrations and its distributions werestudied.The main aerosol sources from which the aerosols in the samples collected came were investigated.The conclusion was drawn preliminarily as follows.The TSP concentrations decreased with height.Over 70% of the aerosol mass were distributed in the fine particle group (d<2.1μm).The top 20 aerosol elements with high concentration are listed from high to low according to their concentrations,and they are S,Fe,Ca,K,A1,Na,Mg,Zn,Cl,Ba,P,Ti,Pb,Mn,As,Cu,V,Br,Cr,and Sb.The aerosol element concentrations decreased with height,too.The mass of volatile elements was mainly distributed in the fine particle group.The ion mass was distributed in the same way as the element mass.From the point of view of contribution to the air aerosols,both anthropogenic and natural sources are important for Beijing.     

ELEMENTAL CONCENTRATIONS AND THEIR SIZE DISTRIBUTIONS OF BEIJING AEROSOL IN JANUARY

Aerosol sampling was carried out at a city centre site and a suburb site in Beijing in January 1983. PIXE (Proton Induced X-ray Emission) compatible cascade impactors were employed. The samples were analysed for 20 elements by PIXE in Fudan University. It has been found that most of the elements have bi-mode size distributions with a gradual progression from mainly coarse mode Ca, Ti and Al to mainly fine mode Zn, As and Pb. Elements Cl, K, S and Si show most obvious bi-mode, of which Si and S are particularly interesting. The concentrations of coarse mode aerosol in the city centre are about 1.4 times as large as that in the suburb for most of the elements, while the concentrations of fine mode aerosol in the city centre differ greatly from that in the suburb and vary significantly among elements, indicating some industrial sources. The enrichment factors of elements indicate that the coal smoke has a large-scale influence in North China.     

Polarimetric Study of the Fine Aerosol Fraction in Beijing

Measurements of aerosol optical characteris- tics were carried out with a Photoelectric Aerosol Nephelometer （PhAN） in Beijing and at Xinglong Obser- vatory, which is located 150 km northeast of Beijing. Aerosol size distributions were retrieved by means of the inverse problem solution. Mean volume size distributions of the fine aerosol fraction were unimodal with the maximum radius in the range 0.11-0.15 pm. Accumula- tion of aerosol matter in the air basin of Beijing takes place mainly due to the growth of particle size, but not their number. A simple optical method to detect aerosol nonsphericity is proposed.     

Aerosol Optical Properties and Radiative Impacts in the Pearl River Delta Region of China during the Dry Season

Aerosol optical properties and direct radiative effects on surface irradiance were examined using seven years(2006–2012)of Cimel sunphotometer data collected at Panyu—the main atmospheric composition monitoring station in the Pearl River Delta(PRD) region of China. During the dry season(October to February), mean values of the aerosol optical depth(AOD)at 550 nm, the ?ngstr?m exponent, and the single scattering albedo at 440 nm(SSA) were 0.54, 1.33 and 0.87, respectively.About 90% of aerosols were dominated by fine-mode strongly absorbing particles. The size distribution was bimodal, with fine-mode particles dominating. The fine mode showed a peak at a radius of 0.12 μm in February and October(~0.10μm~3μm~(-2)). The mean diurnal shortwave direct radiative forcing at the surface, inside the atmosphere(FATM), and at the top of the atmosphere, was-33.4 ± 7.0, 26.1 ± 5.6 and-7.3 ± 2.7 W m~(-2), respectively. The corresponding mean values of aerosol direct shortwave radiative forcing per AOD were-60.0 ± 7.8, 47.3 ± 8.3 and-12.8 ± 3.1 W m~(-2), respectively. Moreover,during the study period, FATMshowed a significant decreasing trend(p 0.01) and SSA increased from 0.87 in 2006 to 0.91 in 2012, suggesting a decreasing trend of absorbing particles being released into the atmosphere. Optical properties and radiative impacts of the absorbing particles can be used to improve the accuracy of inversion algorithms for satellite-based aerosol retrievals in the PRD region and to better constrain the climate effect of aerosols in climate models.     

Seasonal variations of number size distributions and mass concentrations of atmospheric particles in Beijing

Particle number and mass concentrations were measured in Beijing during the winter and summer periods in 2003, together with some other parameters including black carbon (BC) and meteorological conditions. Particle mass concentrations exhibited low seasonality, and the ratio of PM2.5/PM10 in winter was higher than that in summer. Particle number size distribution (PSD) was characterized by four modes and exhibited low seasonality. BC was well correlated with the number and mass concentrations of accumulation and coarse particles, indicating these size particles are related to anthropogenic activities.Particle mass and number concentrations (except ultra-fine and nucleation particles) followed well the trends of 13C concentration for the majority of the day, indicating that most particles were associated with primary emissions. The diurnal number distributions of accumulation and coarse mode particles were characterized by two peaks.     

Atmospheric aerosol characterization in 2010 anomalous summer season in the Moscow region

Daily measurements of atmospheric aerosol characteristics were carried out in Dolgoprudny (Moscow region) in June–August 2010. The particle concentrations at 11 size gradations within the range of 0.01–10 μm and the concentrations of cloud condensation nuclei active at water vapor supersaturation of 0.2–1% were determined. It is shown that the long anticyclonic conditions and the burning of forests and peat bogs resulted in the increase in total aerosol concentration in surface air by more than 1.5 times and in concentrations of particles with the diameter of 0.1–1 μm and > 1 μm by 5 and 10 times, respectively. The fire smoke mainly consisted of the particles with the size of 0.1–3 μm. The particles with the size of more than 5 μm were not observed. The recurrent visibility decrease up to hundreds of meters was caused by the increase in the concentration of particles with the diameter of more than 0.32μm in the air. During the smoke blanketing, the concentration of active condensation nuclei in aerosol increased almost by 20 times that created an opportunity for watering of aerosol particles and formation of the acid smog.     

Physicochemical Transformation and Photochemical Reactions in High-Disperse Substance State: Chemical Decomposition in Aerosols and Thin Films Made from Pesticide Fipronil (Adonis)

A chemical substance being in a high-disperse state (fine aerosol particles and very thin films) in the environment reveals specific chemical and physicochemical features which differ from the processes in a relatively coarse disperse object and, even more, in ordinary liquid and solid “test-tube” assays. The kinetics and the mechanism of the direct and sensitized photochemical destruction of pesticide compound fipronil C₁₂H₄Cl₂F₆N₄OS have been experimented as applied to the aerosol particles ≈0.12–1.3 μm in diameter and thin films ≈0.02–0.6 μm thick on the glass plates. A non-photochemical (“dark”) reaction of fipronil molecules with the OH radicals which spontaneously proceeds in the ambient air was also observed. Quantitative estimations based on experimental results show that the fipronil pollutant, observed in the atmosphere in the form of levitated aerosols, can convert chemically in the above reaction with the OH radicals for a very short time (from several minutes for a particle 2 μm in diameter to 12–24 h for a particle of 20–30 μm). The fipronil residues presented on foliage either in the form of 1–20 μm films or as a group of deposited 2–30 μm aerosols react under sunlight by two photochemical pathways (photooxidation and photodecay). The lifetime of these residues in the ambient conditions is expected to be 11–25 days. Besides, adding a small amount of the Shirvanol 2 sensitizer to the fipronil formulation, one can increase the overall decomposition rate to 8–12 days.     

Applying size segregation to relate the surrounding aerosol pollution to its source

Size segregated sampling of aerosol particles at the coal-fired power station Šoštanj, Slovenia was performed by a newly developed system. In addition, simultaneous sampling of particles was performed at two locations, Velenje and Veliki vrh, chosen on the basis of long term monitoring of SO₂ in the influential area of power plant. The signature of the power plant (e.g. characteristic size distributions of some typical trace elements) was identified. For elements, like As, Mo, Cd and Ga, which are typical for coal combustion, the highest concentrations were observed in the size range between 1 and 4 μm. For Se and sometimes for Ga two modes were identified, first between 0.1 and 0.5 μm and second between 1 and 4 μm. Ratios between the average concentrations of selected elements in fine and coarse particles collected at Veliki vrh (the most influenced location) and Velenje (usually not influenced by the thermo power station) were significantly higher than 1 in the case of Mo and Se for coarse and fine size range, while for As the ratio was higher than 1 for the coarse fraction. Consequently, Mo, Se and As were found as the most important tracers for the emissions from the investigated source. On the basis of the ratios between the concentrations of elements measured in particles at low and high SO₂ concentrations at Veliki vrh, Cd was shown to be a typical tracer as well. Our results definitely showed that size segregated measurements of particles at the source and in the influenced area give more precise information on the influence of source to the surrounding region. It was found that patterns of size distributions for typical trace elements observed at the source are found also in the influenced area, i.e. Veliki vrh.     

Laser desorption/ionization mass spectrometric study of secondary organic aerosol formed from the photooxidation of aromatics

Five aromatic hydrocarbons – benzene, toluene, ethylbenzene, p-xylene and 1,2,4-trimethylbenzene – were selected to investigate the laser desorption/ionization mass spectra of secondary organic aerosols (SOA) resulting from OH-initiated photooxidation of aromatic compounds. The experiments were conducted by irradiating aromatic hydrocarbon/CH₃ONO/NO _X mixtures in a home-made smog chamber. The aerosol time-of-flight mass spectrometer (ATOFMS) was used to measure the aerodynamic size and chemical composition of individual secondary organic aerosol particles in real-time. Experimental results showed that aerosol created by aromatics photooxidation is predominantly in the form of fine particles, which have diameters less than 2.5 μm (i.e. PM2.5), and different aromatic hydrocarbons SOA mass spectra have eight same positive laser desorption/ionization mass spectra peaks: m/z = 18, 29, 43, 44, 46, 57, 67, 77. These mass spectra peaks may come from the fragment ions of the SOA products: oxo-carboxylic acids, aldehydes and ketones, nitrogenated organic compounds, furanoid and aromatic compounds. The possible reaction mechanisms leading to these products were also discussed.     

Peculiarities of seasonal variations of atmospheric aerosol concentration in the surface air of Moscow environs

The seasonal variations of the concentration of particles of different sizes in the atmospheric surface layer are studied on the basis of the data of daily measurements of atmospheric aerosol characteristics in the town of Dolgoprudny (20 km from the center of Moscow) carried out in 2006–2009. It is revealed that the steady variations of monthly mean aerosol concentration are observed within the particle diameter interval of 0.02–1 μm. The annual course of concentration of these particles has two maxima, in February-March and in September–October, and one minimum in June. The concentrations of particles with the size of 0.01–0.02 μm defined by the general atmospheric background and the concentrations of particles of >1 μm associated with the local sources do not have clearly pronounced seasonal variations. It is shown that the regularities of the annual concentration variations of particles with the size of 0.02–1 μm are mainly explained by the sign and value of the lapse rate in the layer up to 925 hPa that indicates the prevalence of the vertical mixing in the processes of aerosol scattering in the surface layer as compared with the horizontal transfer.     

Optical and radiative properties of aerosols during a severe haze episode over the North China Plain in December 2016

The optical and radiative properties of aerosols during a severe haze episode from 15 to 22 December 2016 over Beijing, Shijiazhuang, and Jiaozuo in the North China Plain were analyzed based on the ground-based and satellite data, meteorological observations, and atmospheric environmental monitoring data. The aerosol optical depth at 500 nm was < 0.30 and increased to > 1.4 as the haze pollution developed. The Ångström exponent was > 0.80 for most of the study period. The daily single-scattering albedo was > 0.85 over all of the North China Plain on the most polluted days and was > 0.97 on some particular days. The volumes of fine and coarse mode particles during the haze event were approximately 0.05–0.21 and 0.01–0.43 μm³, respectively—that is, larger than those in the time without haze. The daily absorption aerosol optical depth was about 0.01–0.11 in Beijing, 0.01–0.13 in Shijiazhuang, and 0.01–0.04 in Jiaozuo, and the average absorption Ångström exponent varied between 0.6 and 2.0. The aerosol radiative forcing at the bottom of the atmosphere varied from –23 to –227,–34 to –199, and –29 to –191 W m^–2 for the whole haze period, while the aerosol radiative forcing at the top of the atmosphere varied from –4 to –98, –10 to –51, and –21 to –143 W m^–2 in Beijing, Shijiazhuang, and Jiaozuo, respectively. Satellite observations showed that smoke, polluted dust, and polluted continental components of aerosols may aggravate air pollution during haze episodes. The analysis of the potential source contribution function and concentration-weighted trajectory showed that the contribution from local emissions and pollutants transport from upstream areas were 190–450 and 100–410 μg m^–3, respectively.     

Biogenic and anthropogenic organic matter in aerosol over continental Europe: source characterization in the east Baltic region

An Aerodyne quadruple aerosol mass spectrometer (Q-AMS) has been used to provide on-line measurements of size dependent chemical composition of fine aerosol particles (PM₁) at the Air Pollution Research Station in Preila, Lithuania, representing the east Baltic region. The size dependent chemical composition measurements by AMS have revealed that in marine air masses 118?nm mode organics-containing particles were fresher compared to sulfate-containing particles (295?nm), likely originated as secondary aerosol from forest emissions or produced by primary sea spray over the Baltic Sea. In polluted continental air masses sulfate and organics were highly internally mixed and aged. The mass spectral results indicated that the major components of organic compounds were oxygenated organic species with strong signals at m/z 18, 43, 44 with several specific features. Positive matrix factorization (PMF) of AMS organic mass spectral data has identified three factors: aged oxygenated low-volatility organic aerosol (LV-OOA), less oxygenated semi-volatile organic aerosol (SV-OOA), and biogenic organic aerosol (BGOA) of either terrestrial or marine origin. The measurements were compared with a real-time particulate matter Beta Absorption Monitor (Thermo ESM Andersen) and Micro Orifice Uniform Deposit Impactor (MOUDI) data. The intercomparison showed a good correlation and a stable ratio between PM₁ and PM_2.5 concentrations. A comparison of the on-line Q-AMS data and the off-line MOUDI fine particle (<1???m) data yielded a reasonable agreement in size distributions but not the absolute mass concentrations due to sampling conditions, evaporation of acidic species from sampling substrates and bounce of the particles in the MOUDI.     

2008年北京奥运会期间大气气溶胶物理特征分析

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.     

天空辐射计观测2006年春季北京地区气溶胶光学特性的研究

利用2006年3～5月天空辐射计观测数据反演得到北京地区春季大气气溶胶光学性质参数,包括大气气溶胶光学厚度(0.5μm)、Angstrm指数、单次散射反射比和粒子谱分布特征。结果表明:北京地区春季气溶胶平均光学厚度0.67,Angstrm指数0.54,单次散射比0.88,粒子吸收性质较弱,粒子谱呈双峰形,以粗粒子为主,粗、细模态粒子粒径分别集中在0.17μm和7.7μm左右。相比2004年此次观测期间气溶胶粒径较大,粒子体积浓度较高,散射作用在其消光特性中的比重略有下降。光学厚度日变化呈单峰型,日间单次散射比随时间逐渐递减,Angstrm指数在上午递减趋势明显,午后变得稳定。对同时观测的天空辐射计与CE-318不同波长光学厚度结果进行比较,结果显示两者得到的光学厚度相关性很好,各波长小时平均结果的相对误差小于7%。