A parametric investigation of electrical effects on aerosol scavenging by droplets over large fires

Our nucleation model of strong up-drafts over large fires (such as those ignited by nuclear blasts) show that many droplets in the size range of 1–10 μm are rapidly formed when the cloud becomes supersaturated. In this study we calculate aerosol/droplet collection kernels for electrical parameters commonly seen in cloud air. These kernels, which do not include Brownian diffusion, are used with aged droplet distributions to determine instantaneous scavenging rates of unwettable aerosols with cloud droplets. We find that within a portion of this parameter space the aerosol may be removed from the cloud air with time constants substantially below 1 h over the entire aerosol size range of 0.025–0.5 μm. For much of the parameter space, E-field enhanced attachment of charged aerosol is more rapid than that for Brownian diffusion.The aging of the droplet distribution incorporates the detailed microphysics of nucleation and condensation in a Lagrangian parcel with forced up-draft of 50 m s⁻¹. We assume an initial aerosol distribution that is lognormal about a median radius of 0.05 μm with a geometric standard deviation of 2. Initially there are 10⁶ insoluble aerosol particles per cubic centimeter of air with one-half of them being wettable and the other half being non-wettable.We present our results as a set of curves showing collection kernels and instantaneous scavenging rates vs aerosol radius and electric field strengths. The collection kernel curves are parametrically displayed for droplets of radii 1, 3 and 10 μm and electrical parameters typical of cumulus and thunderstorm clouds. The instantaneous scavenging curve vs aerosol radius is displayed as a function of electrical parameters.     

天津城区大气气溶胶复折射指数的反演及消光贡献分析

气溶胶的复折射指数是直接影响其散射特性和吸收特性的基本物理量之一.为深入研究城市大气气溶胶的复折射指数特征,引入一种具有高时间分辨率优点的反演方法来反演气溶胶复折射指数.依据辐射传输理论,将天津大气边界层观测站观测到的高精度散射系数、吸收系数和数浓度谱分布数据利用查表法代入Mie理论气溶胶粒子群消光计算公式,对大气气溶胶复折射指数进行反演.结果表明:①天津城区2011年4月观测地点0.55 μm波长处的气溶胶复折射指数实部平均值为1.64,虚部平均值为0.015.②气溶胶复折射指数实部和虚部均有明显日变化规律,实部和虚部均与相对湿度呈正相关,与风速呈负相关.③利用反演得到的复折射指数对不同粒径大气气溶胶的消光特性进行计算发现,对散射特性而言,>0.25~1.00 μm粒子对散射系数的贡献率达86%;对吸收特性而言,>0.25~2.50 μm粒子对吸收系数的贡献率为53%,>2.50~32.00 μm粒子对吸收系数的贡献率为47%.研究显示,>0.25~1.00和>1.00~32.00 μm的粒子对吸收系数的贡献率均较高,但对散射系数而言,>0.25~1.00 μm的粒子贡献率较高,因此综合考虑气溶胶散射系数、吸收系数和消光系数,控制>0.25~1.00 μm的气溶胶粒子数浓度可有效改善大气能见度.      

Cloud chemistry at Mt Rigi,Switzerland: Dependence on drop size and relationship to precipitation chemistry

The chemical composition of winter and spring cloud water sampled at 1620 masl elevation on Mt Rigi in central Switzerland was dominated by NO₃⁻, SO₄²⁻, NH₄⁺ and H⁺. A wide range of concentration levels was observed, with maxima of 3700, 1800 and 4600 micronormal for NO₃⁻, SO₄²⁻ and NH₄⁺, respectively. Concentrations at a lower elevation (1030 masl) site on the mountain were higher due to lower cloud liquid water contents and higher pollutant levels at that site. The lowest pH observed was 2.95; large concentrations of NH₃ in the region prevented pH values from falling even lower. A comparison of simultaneously sampled cloud water and precipitation revealed much higher concentrations for most species in the cloud water, except in one case of extreme precipitation riming when the concentrations in the two phases converged. An exception to the pattern was H⁺; at times the precipitation was more acidic than the cloud water. The chemical composition of the cloud drops varied with drop size. Drops smaller than 10 μm diameter were enriched in NO₃⁻, SO₄²⁻ and NH₄⁺ relative to larger drops. Since the larger drops are the ones most effeciently captured by snow crystals, knowledge of their composition is essential to understanding the chemical implications of accretional growth of precipitation.     

Chemical composition differences in fog and cloud droplets of different sizes

The distribution of acidity and solute concentration among the various droplet sizes in a fog or cloud and the effect of the evaporation-condensation cycle on the composition and size distribution of atmospheric aerosol is studied. Significant total solute concentration differences can occur in aqueous droplets inside a fog or cloud. For the fog simulated here, during the period of dense fog, the solute concentration in droplets larger than 10 μm diameter increased with size, in such a way that droplets of diameter 20 μm attain a solute concentration that is a factor of 3.6 larger than that in the 10 μm droplets. Droplets on which most of the liquid water condenses have access to most of the reacting medium for in situ S(IV) oxidation and are therefore preferentially enriched in sulfate. The gas and aqueous-phase chemical processes result in an increase of the total solute mass concentration nonuniform over the droplet spectrum for a mature fog. These chemical processes tend to decrease the total solute mass concentration differences among the various droplet sizes. Low cooling rates of the system also tend to decrease these concentration differences while high cooling rates have exactly the opposite effect. The mass/size distribution of the condensation nuclie influences quantitatively, but not qualitatively, the above concentration differences.     

黄山山底大气气溶胶数浓度日变化

利用美国MSP公司生产的宽范围粒径谱仪(WPS)于2011年5月至9月在黄山山底(寨西)采集的气溶胶观测数据,分析了黄山山底大气气溶胶数浓度的日变化特征.结果表明晴天气溶胶数浓度日变化特征明显,气溶胶粒子总数浓度在6:00,12:00和18:00达到峰值.人为活动,湍流混合及山谷风是影响黄山山底气溶胶日变化的主要因素.剔除交通污染时段后,气溶胶粒子数平均浓度减少319个/cm3,即减少12.17%.其中,0.01~0.02μm,0.02~0.05μm,0.05~0.1μm,0.1~0.5μm,0.5~1.0μm,1.0~2.5μm粒径段气溶胶粒子数浓度分别降低了31.32%,20.29%,6.59%,7.49%,1.23%,2.51%.机动车尾气排放对0.01~0.05μm粒径段气溶胶的影响最明显,其气溶胶浓度降低百分比为25.81%.     

一次对流过程对气溶胶清除和再生过程的影响

利用中尺度天气预报和研究模式(WRF)对2007年4月23～24日广东省发生的一次飑线过程进行了模拟,研究了水凝物粒子对气溶胶的清除过程、液滴蒸发引起的气溶胶再生过程以及动力输送作用对气溶胶数浓度的影响.结果表明,降水与近地层气溶胶数浓度的变化呈负相关关系.综合对比各水凝物种类的碰撞清除率和核化清除率,发现云滴核化过程...     

Project aguila: In situ measurements of Mexico City air pollution by a research aircraft

Measurements of aerosol concentrations, chemical species and meteorological quantities in the air above Mexico City were obtained from an instrumented research aircraft. Concentrations of particles in the size range between 0.12 and 3.12 μm were nearly invariant with height, and typical values were of the order of 5000 cm⁻³. However, particles smaller than 0.12 μm were confined to the lowest few hundred meters of the atmosphere until the morning temperature inversion dissipated, after which time those particles, together with newly formed particles created by secondary processes, mixed to a greater height above the city. Total particle concentrations near the surface attained values in excess of 60,000 cm⁻³. An examination of the corresponding profiles of SO₂ suggests that combustion processes are likely sources for the additional small particles.     

半干旱区沙尘天气对0010～10 μm沙尘气溶胶分布的影响

利用WPS粒子谱仪对内蒙古朱日和背景天气及沙尘天气的气溶胶数浓度进行了观测,研究了不同天气背景下沙尘气溶胶数浓度及谱分布特征. 结果表明:在背景天气和沙尘天气下,0.010～0.020,0.021～0.100,0.101～1.000,1.001～2.500 μm等粒径段的气溶胶数浓度差别较大;沙尘天气对各粒径段,尤其是大于1.0 μm的气溶胶数浓度影响较大,沙尘暴过程中1.001～2.500 μm粒径段的气溶胶数浓度约为背景天气的35倍;各粒径段气溶胶数浓度在不同天气背景下的日变化规律有所不同,受气象要素的影响较大. 对沙尘气溶胶谱分布的分析可知,沙尘暴发生前后1 h的沙尘气溶胶谱型均符合Lorentz分布,背景天气下同时段的沙尘气溶胶谱型也符合Lorentz分布;沙尘天气下沙尘气溶胶谱型在沙尘暴发生前1 h的主峰值比背景天气高1个数量级,沙尘暴发生后1 h的峰值半径明显移向大粒子.      

Characteristics of secondary inorganic aerosol and sulfate species in size-fractionated aerosol particles in Shanghai

Sulfate, nitrate and ammonium(SNA) are the dominant species in secondary inorganic aerosol, and are considered an important factor in regional haze formation. Size-fractionated aerosol particles for a whole year were collected to study the size distribution of SNA as well as their chemical species in Shanghai. SNA mainly accumulated in fine particles and the highest average ratio of SNA to particulate matter(PM) was observed to be 47% in the fine size fraction(0.49–0.95 μm). Higher sulfur oxidation ratio and nitrogen oxidation ratio values were observed in PM of fine size less than 0.95 μm. Ion balance calculations indicated that more secondary sulfate and nitrate would be generated in PM of fine size(0.49–0.95 μm). Sulfur K-edge X-ray absorption near-edge structure(XANES) spectra of typical samples were analyzed. Results revealed that sulfur mainly existed as sulfate with a proportion(atomic basis) more than 73% in all size of PM and even higher at 90% in fine particles. Sulfate mainly existed as(NH4)2SO4 and gypsum in PM of Shanghai. Compared to non-haze days, a dramatic increase of(NH4)2SO4 content was found in fine particles on haze days only, which suggested the promoting impact of(NH4)2SO4 on haze formation. According to the result of air mass backward trajectory analysis, more(NH4)2SO4 would be generated during the periods of air mass stagnation. Based on XANES, analysis of sulfate species in size-fractionated aerosol particles can be an effective way to evaluate the impact of sulfate aerosols on regional haze formation.     

A theoretical determination of the collection rates of aerosol particles by falling ice crystal plates and columns

A theoretical model for the removal of aerosol particles by falling columnar ice crystals is compared to the model results for the removal of aerosol particles by falling planar ice crystals. These results incorporate gravitational, inertial, electrostatic, thermophoretic, diffusiophoretic, and Brownian diffusion mechanisms. Scavenging rates for columnar and planar ice crystals are computed for aerosol particles ranging from 0.001 to 10 μm in radius. The results show that planar ice crystals have greater collection efficiencies than the columnar ice crystals.     

珠江三角洲地区大气中的粒子污染

从珠江三角洲地区航测发现,直径小于1μm的气溶胶粒子每毫升可达几万到几十万个,这类小粒子能沉积在肺泡中,对人的健康危害较大,而它们对能见度影响较小。这类细粒子的来源,除排放源以外,气态污染物的转化也是细粒子二次污染的重要来源。野外烟雾箱模拟实验表明,珠江三角洲二氧化硫转化率最高达12.7%/小时,影响SO₂转化的因素是SO₂起始浓度、相对湿度和光照强度。经估算,珠江三角洲地区现有火电站与拟建火电站所排放的SO₂经转化,单是形成的硫酸盐细粒子(≤1μm)污染浓度,约为每毫升几万个,这是一个不容忽视的问题。对广州城市大气污染物有机无机成分的分析表明,就对人体健康而言,广州市气溶胶中有机成分的污染占主导地位。      

Submicron aerosol size distributions measured over the tropical and South Pacific

Size distributions of aerosol particles in the radius range of 0.006–0.53 μm were measured over the Pacific Ocean along the 150° longitude from about 20°N to 55°S. Throughout the tropical trade wind region, the size distribution of fine particles was relatively stable and exhibited a double-peaked characteristic with one peak at about 0.1 μm and the other in the 0.02–0.04 μm region, separated by a minimum at about 0.06 μm. The total concentrations of particles were in the 150–300 cm⁻³ range with 60–150 cm⁻³ residing in the accumulation mode (0.06<r<0.5 μm). South of the trade wind region, the measured size distributions and meteorological conditions were more diverse. Periods with very low concentrations in the accumulation mode were associated with regions of large-scale precipitation. Large increases in the number of nucleation mode particles were found in air masses with low concentrations of particles in the accumulation mode.     

新疆干旱区气溶胶间接效应区域性分析

利用MODIS气溶胶和云资料以及实测的降水数据,可从宏观角度分析新疆区域气溶胶时空分布特征,研究气溶胶与云和降水之间的相互影响关系.结果表明：近十年来受区域暖-干趋势的转变影响,新疆地区气溶胶光学厚度空间分布呈现显著的区域性和季节性差异;南疆地区气溶胶光学厚度整体高于北疆地区,春、夏高,秋、冬低,整体呈现增加趋势,其中,北疆地区气溶胶光学厚度变化程度相对较为显著;受气候变化和颗粒粒径差异影响,新疆干旱区云光学厚度与气溶胶光学厚度呈负相关变化趋势,相关系数北疆地区高于南疆地区;云水路径受温度、湿度影响较大,对气溶胶光学厚度的变化的敏感程度北疆大于南疆,夏季最高,冬季最低;气溶胶光学厚度与云滴粒子有效半径关系复杂,受水汽影响较大,在云层含水量较低的情况下,云滴粒子有效半径与气溶胶光学厚度呈负相关,说明在干燥地区或季节,气溶胶的增加,抑制云滴粒子的增长;整体来看,新疆干旱区气溶胶的增加抑制了区域降水的形成.     

Size distribution measurements of suspended particulate matter in Ponce,Puerto Rico

Size distribution measurements using a high volume sampler with a cascade impactor have been obtained for the city of Ponce, Puerto Rico from 1985 to 1987. The data indicate that the concentration of particles < 2 μm in diameter remained constant during the sampling period while the concentration of particles > 7 μm showed time variations. Aerosol from this area is greatly composed of particles > 7 μm in diameter, they accounted for over 45% of the Total Suspended Particulate (TSP) of this area. Over 75% of the aerosol concentration is from particles > 3.3 μm, approximately only 20% of the aerosol concentration is from particles < 2 μm in diameter. A linear relationship was observed between the different particle size and the TSP, except for those particles < 1.1 μm in size. The size distribution and its time variation are explained in terms of local sources such as agriculatural burning, natural contributions and industrial activities, as well as contribution from the Sahara haze that crosses the Atlantic from Africa and reaches the Caribbean region during the summer.     

上海大气颗粒物中糖类的组成、粒径分布及来源

为更好地理解大气颗粒物中糖类的来源及其环境影响,利用微孔撞击式采样器(MOUDI)采集了上海市宝山区2012年11月—2013年8月四季节代表性时段18 μm以下11个不同粒径段的大气颗粒物样品,利用硅烷化衍生和GC-MS对10种脱水糖、单糖和糖醇类化合物进行了分析. 结果表明:上海大气颗粒物中所检测的10种糖类化合物的质量浓度之和在春、夏、秋、冬四季采样期的平均值分别为120.3、104.0、292.9和206.0 ng/m3,脱水糖在秋、冬季占主导地位,单糖和糖醇的质量浓度在冬季最低. 绝大部分脱水糖存在于粒径≤1.8 μm的颗粒中,冬、夏季质量浓度最高的粒径段(峰值粒径)为>0.32~0.56 μm,而春、秋季峰值粒径为>0.56~1.0 μm. 单糖和糖醇类化合物在春、夏季时主要存在于粒径>1.8 μm的颗粒中,而秋、冬季时在粒径≤1.8 μm的颗粒中质量浓度较高. 应用PMF(正定矩阵因子分析法)解析出了大气颗粒物中糖类的3个来源——生物质燃烧、植物源土壤有机质和微生物源土壤有机质. 脱水糖全部来源于生物质燃烧,单糖主要来源于植物源土壤有机质,而糖醇主要来源于微生物源土壤有机质;秋、冬季时生物质燃烧对山梨糖醇之外的单糖和糖醇有较大贡献.      

山西夏季气溶胶空间分布飞机观测研究

以搭载了多种气溶胶观测仪器的飞机为观测平台,在2013年夏季首次对山西中部地区霾日及晴空大气气溶胶空间分布特性进行了观测,得到气溶胶粒子数浓度和尺度的垂直分布廓线以及不同高度气溶胶粒子谱分布特征.研究发现,山西夏季非降水天气条件下气溶胶粒子以核模态和积聚模态的细粒子为主,粗粒子很少.霾日气溶胶数浓度是晴空的2~3倍,主要是核模态的小粒子;气溶胶粒子数浓度随着高度逐渐减小,低空存在气溶胶累积区,逆温层的存在是导致气溶胶累积区形成的主要原因;气溶胶粒子尺度随高度增加,大粒子主要分布在2500m以上的高空;不同高度上的气溶胶粒子谱均呈双峰或三峰分布,谱型基本一致,从近地面到5000m高空,气溶胶粒子谱随高度的增加略有展宽.观测区域气团后向轨迹模拟结果显示,4000m以上高空气溶胶粒子主要是从中国西北地区远距离输送而来,3000m以下气溶胶粒子则主要来源于近地面排放.     

基于气溶胶光学特性的颗粒物来源分析

为初步探讨利用气溶胶光学指标判别污染物来源的适用性,选取天津市冬季一次重污染过程（2017年11月17—21日）,对气溶胶的七波段吸收系数、三波段散射系数及其化学组分进行在线观测及分析,研究气溶胶光学特性的变化,并结合化学组分定性分析污染过程不同阶段的污染来源.结果表明:SSA（单散射反照率）可以从散射性组分和吸光性组分对消光贡献的变化判断污染来源.污染积累期,颗粒物中散射性组分（SO₄2-、NO₃-、NH₄+）的增幅高于吸光性组分EC（元素碳）,导致污染积累期的SSA值高于污染前期和污染消散期,说明污染积累期存在较明显的二次转化过程.SAE（散射波长指数）可以从粒径角度推断污染来源.此次观测的污染积累期SAE值呈较明显的下降趋势,说明在细粒径段（2.5 μm以下）颗粒物粒径有增大的趋势,这主要与颗粒物中无机盐的吸湿增长及颗粒物之间的碰并有关.AAE（吸收波长指数）在一定程度上可以指示吸光颗粒物的类型.污染前期,BrC（棕色碳）在370、470 nm处对光吸收的贡献率分别为50.7%、33.8%;同期PM_2.5中ρ（Cl-）、ρ（K+）同步升高,卫星遥感显示,观测点周围有大量火点出现,推测主要受祭祖活动的影响.研究显示,气溶胶光学指标能够从散射性组分和吸光性组分对消光贡献变化、粒径变化、吸光颗粒物类型角度定性解析一部分污染来源,但其对于燃煤源和机动车等重要源类的指示作用还有待进一步研究.      

南京地区大气气溶胶及水溶性无机离子特征分析

于2010~2011年在南京市城郊两个采样点收集了气溶胶样品,并利用离子色谱(IC)法分析了其中的水溶性无机离子成分.结果表明,采样期间除了夏季,其他3个季节南京城郊气溶胶污染都较严重.南京城郊气溶胶谱分布特征基本在0.65~2.1μm和5.8~9μm粒径段出现峰值.PM2.5与能见度的相关性很大.城郊离子总质量浓度均是春冬季高于夏秋季,四季阴离子质量浓度明显高于阳离子,且这一特征在细粒子上表现明显.水溶性离子在气溶胶中所占比例是夏秋冬季城区高于郊区.南京城郊NO3-/SO42-年均值表明采样期间燃煤仍然是主要污染源,且该比值夏季最低,冬季最高.NH4+、K+、NO3-和SO42-主要富集在细粒子上;Na+、Cl-和NO2-在粗粒子和细粒子上都有富集;Ca2+、Mg2+和F-主要在粗粒子上富集.因子分析(FA)的方法表明南京城区气溶胶主要有3个来源.     

Aerosol-soil fractionation for Namib Desert samples

Four soil samples, collected in the central Namib Desert, were fractionated by dry sieving and aerosol generation into 16 size fractions in the range 0.15–300 μm diameter. The mass-size function of each soil and the dust (mineral aerosol) generated from the soil were studied. Due to the preferential lifting of smaller soil particles by the air stream, the soil underwent strong physical fractionation resulting in the bulk of the dust being found in the range of 1.3–10.3 μm, whereas the bulk of the soil was found in the range 63–300 μm. The concentrations of 11 elements in eight soil size fractions (from <45 to >300 μm) obtained by dry sieving were measured by X-ray fluorescence analysis while the concentration for these elements in eight size ranges (from <0.15 to >10.3 μm) obtained by aerosol generation were determined by particle-induced X-ray emission. The concentrations of the elements Al, Si, K, Rb and Sr were found to vary by less than a factor of two throughout the particle size range studied. However, the concentration of the elements Ca, Ti, Mn, Fe, Y and Zr increased when the particle size decreased below 150 μm to reach a maximum around 63-45 μm and then to decrease. The concentrations of the elements in the generated aerosol particles were found to be more similar to those in the bulk soil than any particular size fraction. For the aerosol size fraction, elemental enrichment factors were calculated with respect to the composition of average crustal rock, average soil, the bulk Namib soil and the small size fraction of the Namib soil. For several elements, the enrichment factors varied quite significantly, depending on the choice of the reference material. The elemental ratios in the mineral aerosol were also compared to those in the atmospheric aerosol from the Namib Desert. It was confirmed that there is a marine contribution for S, Cl and Sr in the Namib natural aerosol. The composition of the mineral aerosol generated in this study should be useful in source apportionment studies for the Namib Desert and sorrounding regions.