南京雾过程对大气气溶胶谱分布及化学组成的影响

为探究南京地区雾过程对气溶胶粒子化学组成和尺度分布的影响,在2017年冬季的雾观测中平行收集了3级分档雾水和分粒径气溶胶样品,并对雾微物理量与气溶胶谱分布、3级分档雾水与雾前、雾中、雾后分粒径气溶胶化学组成对比分析。结果表明,2017年冬季南京第1次雾过程的雾滴液态水含量随粒径分布为不对称“V”型,最低值位于7μm处,第2次雾过程的雾滴液态水含量随粒径分布为3峰型,峰值分别位于5,15,21.5μm处。在雾形成、发展阶段,粒径<0.33μm的气溶胶质量浓度降低,粒径0.38μm气溶胶质量浓度升高,雾成熟阶段,气溶胶粒子质量浓度在全粒径段均达到最低,粒径0.38μm的气溶胶质量浓度大幅降低,与雾前相比,雾后气溶胶质量浓度峰值向大粒径方向移动。雾前,气溶胶水溶性离子组分富集在粒径<0.43μm的小粒子中,随着雾过程进行,成核作用和吸湿增长使得水溶性离子向较大粒径段富集。雾中新生成的气溶胶随着雾滴的蒸发被释放,导致雾后NO₃^-、SO₄^2-和NH₄⁺浓度升高。较小粒径的气溶胶中和率更高,雾形成初期的新生雾滴酸性较强,随着雾过程的进行逐渐中和,雾水pH值逐渐升高。     

石家庄地区雾霾天气下云滴和云凝结核的分布特征

2009年5~10月在石家庄地区对雾霾天气下的近地面到高空的云雾滴和云凝结核(CCN)进行了7架次飞机探测.利用PMS云粒子测量仪器、机载温湿仪和连续气流纵向热梯度云凝结核仪获得的云雾粒子和云凝结核(CCN)探测资料,分析了层积云(Sc)和高积云(Ac)中云粒子浓度、液态含水量、粒子算术平均直径和粒子有效平均直径的垂直分布特征;分析了CCN垂直和水平分布特征以及谱分布.结果表明雾霾天气状况下,云滴数浓度在102个/cm3量级上.高云粒子粒径总体大于低云粒子.云含水量平均值范围为0.03~0.14g/m3;地面到600 m高度内, CCN值的平均值为3034cm-3(过饱和度S=0.3%).对CCN的活化谱进行拟合表明石家庄属于典型大陆性核谱,云对CCN有消耗作用,逆温层的存在使得该区CCN浓度累积增加.     

华南高山背景地区黑碳云内清除特征

基于2020年南岭背景高山地区的3个典型云事件,利用地用逆流虚拟撞击器采集云中颗粒物,结合单颗粒黑碳光度计和激光雾滴谱仪分析黑碳浓度及云参数特征,探讨黑碳云内清除率及其影响因素.结果表明：进入云内的黑碳约占整体的20%,而云中含黑碳云滴的占比（4.67%）则少于含黑碳间隙颗粒的占比（15.31%）;黑碳的分粒径质量清除率和数量清除率接近,变化范围均为28%~59%;高液态含水量和云滴数浓度有利于黑碳云内清除率的增加,而黑碳云内清除率会随黑碳总浓度的增加而降低,各因素对于黑碳云内清除的影响由大到小为：云滴数浓度>液态含水量>总黑碳浓度.     

Multiphase chemistry in a microphysical radiation fog model—A numerical study

A microphysical radiation fog model is coupled with a detailed chemistry module to simulate chemical reactions in the gas phase and in fog water during a radiation fog event. In the chemical part of the model the microphysical particle spectrum is subdivided into three size classes corresponding to non-activated aerosol particles, small and large fog droplets. Chemical reactions in the liquid phase are separately calculated in the small and in the large droplet size class. The impact of the chemical constitution of activated aerosols on fogwater chemistry is considered in the model simulations. The mass transfer of chemical species between the gas phase and the two liquid phases is treated in detail by solving the corresponding coupled differential equation system. The model also accounts for concentration changes of gas-phase and aqueous-phase chemical species which are induced by turbulence, gravitational settling and by evaporation/condensation processes.Numerical results demonstrate that fogwater chemistry is strongly controlled by dynamic processes, i.e. the vertical growth of the fog, turbulent mixing processes and the gravitational settling of the particles. The concentrations of aqueous-phase chemical species are different in the two droplet size classes. Reactands with lower water solubility are mainly found in the large droplet size class because the characteristic time for their mass transfer from the gas phase into the liquid phase is essentially longer than the characteristic time for the formation of large fog droplets. Species with high water solubility are rapidly transferred into the small fog droplets and are then washed out by wet deposition before these particles grow further to form large droplets. Thus, the concentrations of the major ions (NO₃⁻, NH₄⁺) are much higher in small than in large droplets, yielding distinctly lower pH values of the small particles. In the present study the reaction of sulfur with H₂O₂ and the Fe(III)-catalysed autoxidation of S(IV) are the major S(VI) producing mechanisms in fog water. Most of the time the sulfur oxidation rates are higher in the large than in the small droplets. Fogwater deposition by gravitational settling occurs mainly in the large droplet size class. However, since in the small droplets the concentrations of chemical species with very good water solubility are relatively high, in both droplet size classes the total wet deposition of these reactands is of the same order of magnitude.     

南京2013年冬季三级分粒径雾水化学特征

为研究南京冬季不同粒径雾滴的化学成分的特征,利用three-stage CASCC主动式分档雾水采集器,于2013年12月7日~12月9日南京郊区发生浓雾期间,分时段采集三级分档雾水样本,分档粒径为4~16μm(三级)、16~22μm(二级)、>22μm(一级),共计23个分档雾水样本;用瑞士万通850professional IC型色谱仪器测定水溶性阴、阳离子浓度,分析探讨了三级分粒径雾水中阴、阳离子组分的分布特征,不同粒径雾滴中阴、阳离子浓度的相关性,雾水离子浓度与污染气体以及微物理之间的关系.结果表明,南京雾水的pH值多呈酸性,雾水中的各离子成分分布都与雾滴的大小存在着尺度依赖性关系,小雾滴与大雾滴相比,小雾滴中主要离子成分浓度(NH4+,NO3-,SO42-)高、pH值小且电导率(EC)值高.同时南京雾水中的各离子浓度呈现出夜间高白天低.统计分析显示,南京雾过程中雾水组分的变化,主要源于污染源的贡献差异.结合雾滴谱和污染气体资料分析得出,雾水化学组成的变化与微物理特征以及空气中污染气体有关.     

蓬莱19-3原油水下溢油的模拟实验

把握水下溢油时油滴粒径的分布规律是研究溢油行为和归宿的前提,也是水下溢油事故有效应急处置的重要依据。本研究采用自制的1 m×1 m×2 m（长×宽×高）的水下溢油模拟实验装置开展蓬莱19-3原油的水下溢油模拟实验,以油滴体积分布和油滴体积中值粒径为考察指标,评估了水下溢油喷口直径和喷射速度对油滴破碎形成的油滴粒径分布的影响。结果表明,不同粒径油滴体积分布总体上表现为低于100 μm和高于700 μm的油滴粒径体积占比较小,油滴粒径分布主要集中在100 μm~700 μm之间,体积比最高点位置根据喷射条件的不同而有所偏移。喷口直径保持不变时,随着喷射速度增大,小粒径油滴所占体积逐渐增大,大粒径油滴体积比减小。油滴体积中值粒径随喷射速度的增加而减小,相对体积中值粒径与喷射流量经对数变换后呈线性相关关系。本研究结果可为水下溢油行为轨迹的预测提供重要依据。     

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.     

On the drop and aerosol size dependence of aqueous sulfate formation in a continental cumulus cloud

An entraining air parcel model including microphysical and chemical processes is used to investigate the drop size dependence of pollutant concentrations in a growing cloud under continental background conditions. For the calculation of the chemical processes, the drop size of the cloud drops and their initial dry particle size before activation is taken into account. The size dependence of the pollutant concentration in drops smaller than 8 μm radius is mainly influenced by the activation and fast condensational growth of recently entrained particles. In drops larger than 20 μm radius the main process influencing the drop size dependence of the pollutant concentration is coalescence between drops. The size dependence in drops between 8 and 20 μm radius is determined by the drops activated at the cloud base and the drops growing on particles that are entrained at higher altitudes, the influence of the latter rapidly increasing with height. Drops that are growing on large particles are polluted with initital aerosol matter to such an extent that sulfate production by oxidation is not significant in them. In drops growing on small particles the initial aerosol load has relatively little influence on the chemical processes in the drop. Oxidation of S(IV), especially by ozone, takes place mainly in these drops. The dependence of chemical processes of initial dryk particle size holds throughout the most of the cloud, until coalescence starts playing a role. If the cloud evaporates before producing precipitation-sized drops, the increase of aerosol mass due to cloud chemical processes is found to have taken place in the aerosol accumulation mode. If precipitation-sized drops were produced during the cloud stage, the soluble volume fraction of the aerosol matter has increased throughout the aerosol size distribution, but mainly in the accumulation mode.     

南京2007年12月持续雾霾过程的大气消光特性

2007年南京冬季雾外场综合试验期间,雾、霾交替持续的最长时间达100 h以上。利用大气气溶胶粒子和雾滴数浓度尺度谱分布、能见度、相对湿度等同步观测资料,从Mie散射理论出发,研究了雾、霾不同阶段大气消光特征,重点分析了大气气溶胶粒子和雾滴在雾、霾持续和转化过程中的消光作用。结果表明,雾、霾过程不同阶段平均能见度的大小关系为：雾<湿霾<霾~轻雾。平均而言,雾阶段雾滴和气溶胶粒子的消光作用相当,其中,雾滴消光波动幅度大于气溶胶粒子消光,能见度的变化趋势主要由雾滴的消光决定。湿霾、霾和轻雾阶段的消光主要由气溶胶粒子造成。湿霾阶段的低能见度是由于大量积聚模态的气溶胶粒子在较高相对湿度环境中吸湿增长所致。霾阶段气溶胶粒子数浓度达到最大,核模态粒子占总数浓度的80%左右,是导致该阶段能见度较低的主要原因。轻雾阶段气溶胶粒子的消光系数最小,但雾滴可提供10%~15%的消光贡献,导致能见度与霾阶段相当。     

A preliminary comparison of atmospheric aerosols in urban and non-urban areas in Nanjing,China

Using a 10-stage cascade impactor, atmospheric aerosols were collected from urban and non-urban areas in Nanjing, China. The shapes of average mass distribution were multimodal for both the urban and non-urban samples. The average mass concentration of atmospheric aerosols in the industrial/agricultural area was larger than in city center and natural park areas. The mass median diameter (MMD) were 0.80 μm, 0.51 μm and 0.46 μm for the natural park, city center and industrial/agricultural samples, respectively. In both the urban and non-urban areas, the particles in accumulation and coarse modes were the main contributors to total mass concentration, the particles in Aitken nuclei mode were only a few percent of total mass.     

庐山三级分档雾水化学特征的对比分析

为研究庐山冬季不同粒径雾滴化学成分特征,于2015年和2016年在庐山开展冬季云雾物理化学特征的很高综合观测实验,利用主动式分档雾水采集器（three-stage CASCC）共采集44组3级粒径雾滴的雾水样品,其分档空气动力学直径为4~16μm（S3级）,16~22μm（S2级）和>22μm（S1级）.用850professional IC型色谱仪（瑞士万通）分析雾水中的水溶性离子浓度,讨论3级分档雾水化学特征和不同粒径雾水中各离子组分的来源及相关性.结果表明,2015年和2016年庐山冬季3级雾水多呈酸性,2016年酸性更强,pH值与雾滴的粒径大小有依赖性关系,4~16μm的小雾滴酸性更强.雾水中主要离子有Ca²⁺,NH₄⁺,SO₄^2-,NO₃^-和Cl^-.NH₄⁺,SO₄^2-,NO₃^-主要集中在4~16μm的小雾滴中,受海洋和土壤源的影响比较小,主要是人为活动所导致,2015年雾水Cl^-主要受人为源的影响,2016年人为输入显著降低,主要受海洋源影响.Mg²⁺,Ca²⁺主要集中在>22μm的大雾滴中.SO₂、NO_x排放逐年降低导致2016年雾水中SO₄^2-和NO₃^-浓度明显小于2015年.     

Agglomeration of dust in convective clouds initialized by nuclear bursts

Convective clouds initialized by nuclear bursts are modeled using a two-dimensional axisymmetric cloud model. Dust transport through the atmosphere is studied using five different sizes ranging from 1 to 10,000 μm in diameter. Dust is transported in the model domain by advection and sedimentation. Water is allowed to condense onto dust particles in regions of supersaturation in the cloud. The agglomeration of dust particles resulting from the collision of different size dust particles is modeled. The evolution of the dust mass spectrum due to agglomeration is modeled using a numerical scheme which is mass conserving and has low implicit diffusion. Agglomeration moves mass from the small particles with very small fall velocity to the larger sizes which fall to the ground more readily. Results indicate that the dust fallout can be increased significantly due to this process. In preliminary runs using stable and unstable environmental soundings, at 30 min after detonation the total dust in the domain was 11 and 30%, respectively, less than a control case without agglomeration.     

Determining the acidity and chemical composition of fog,haze and cloud droplets in Israel

The chemistry and acidity of individual droplets were analyzed in samples of fog, haze and cloud collected at Tel Aviv University on the Mediterranean seacoast and at the top of Mt Meron and of Mt Carmel in northern Israel. Acidity was measured using pH paper in a cascade impactor. The characteristics of droplets and interstitial particles 0.3–20.0 μm in size were identified using microspot and electron microscopy techniques.The results revealed the following: (1) the aerosols in the micrometer and sub-micrometer range were mostly very acidic droplets, with pH as low as 2.0, caused by the presence of sulfuric acid; (2) lower acidity was associated with an increase in droplet size, due to dilution by condensation or nucleation scavenging of mineral dust, i.e. gypsum, calcite and dolomite; (3) both acidic and alkaline droplets contained significant amounts of sulfur; and (4) the alkaline droplets contained minerals and salt solutions of Na₂SO₄, CaSO₄, or NaCl.     

西安市两次雾霾期间气象要素和气溶胶特性分析

利用气象要素和气溶胶观测资料,分析了西安市2013年12月17~25日、2014年2月20~26日两次雾霾过程的气象要素风、温、湿变化,气溶胶质量浓度、粒子谱分布及散射系数的变化及其在雾霾天气的形成、发展、维持与变化中的作用.结果表明:APS观测的粒子谱变化表明,雾霾过程中,粒径在0.5~0.835μm之间的粒子的数浓度增加最明显,雾霾后,3.5μm粒子的数浓度下降显著;SMPS观测的粒子谱变化表明,霾过程中细粒子的数浓度主要集中在30~300nm,且具有明显的日变化特征,08:00~14:00、18:00~02:00为数浓度的大值时段,细粒子段污染物浓度的增加主要是由粒径大于140nm以上的粒子引起的.散射系数的增加与粒径小于1.0mm粒子的数浓度增加有关,也是雾霾期间能见度恶化的重要原因之一.     

2009年夏季黄山云雾水化学特征及来源分析

利用09年夏季在黄山光明顶气象站采集的25个云雾水样本及气象站常规资料,分析了云雾过程雾水的化学特征、污染来源与微物理特性.结果表明,观测期间云雾水呈弱酸性,平均值pH值为6.4,主要的离子浓度由大到小排列为:SO42->NH4+>Ca2+>NO3->Na+>Cl-,表明二次污染物对黄山云雾水的贡献较大.统计分析显示,各云雾过程中雾水组分变化,主要缘于不同云雾过程中污染源与海洋源的贡献率不同.结合后向轨迹进一步分析显示,影响气团主要来源于海洋和周边地区,不同气团影响下雾水离子组分及云雾微物理特征差别明显.     

新OG系统旋流脱水器气液分离特性数值研究

根据旋流脱水器的内部流动特性,基于欧拉-拉格朗日方法,对旋流脱水器内部气液两相流动进行了数值计算和分析,研究了液滴直径、进口质量含气率和湍流扩散效应对流场分布、脱水效率、出口质量含气率和出口液滴粒度分布的影响.结果表明：当质量流量一定时,旋流脱水器进出口压降随着进口质量含气率的增加而显著提高.对于单一直径的液滴,在不考虑湍流扩散效应的情况下,脱水效率随进口质量含气率的增加而增加.当考虑湍流扩散效应时,对于直径较小的液滴（0.1~1μm）,这种规律刚好是相反的,连续相速度的增加提升了湍流扩散速度,使湍流运动更加紊乱,但脱水效率高于不考虑湍流扩散效应时的计算结果.在混合粒径条件下,随着进口质量含气率的增加,脱水效率和出口质量含气率增加,计算表明湍流扩散效应有利于混合直径液滴的分离.随着进口质量含气率的增加,液滴质量分数的峰值逐渐向小粒径方向移动,粒径分布范围逐渐减小.     

SO2 oxidation in an entraining cloud model with explicit microphysics

A model of the chemical evolution of the droplets in a hill-cap cloud is presented. The chemistry of individual droplets forming on cloud condensation nuclei of differing size and chemical composition is considered, and the take-up of species from the gas phase by the droplets is treated explicity for the droplet population. Oxidation of S(IV) dissolved in cloud droplets is assumed to be dominated by hydrogen peroxide and ozone.Hydrogen peroxide is normally found to be the dominant oxidant for the oxidation of sulphur dioxide (except in the presence of substantial concentrations of ammonia gas, which increases droplet pH and the contribution made by the oxidant ozone). The entrainment of hydrogen peroxide from above the cloud top increases the amount of sulphate produced in conditions where the reaction is otherwise oxidant limited by the availability hydrogen peroxide. These conditions occur when there are high concentrations of sulphur dioxide accompanied by low cloudwater pH values.Within droplets formed on sodium chloride aerosol, reduced levels of acidity lead to an increase in sulphate production as a result of an enhanced reaction between SO₂ and the oxidant ozone. This results in an overall higher increase in cloudwater sulphate than would be expected assuming an even distribution of all reactants amongst the droplets. In addition, concentrations of the hydrogen sulphite ion predicted to occur in the cloudwater can be substantially in excess of those predicted from the bulk cloudwater pH. This is consistent with recent observations.     

2×350 MW燃煤发电机组主烟道脱硫废水蒸发数值模拟

针对某2×350 MW燃煤发电机组主烟道脱硫废水蒸发过程进行了CFD数值模拟,分析了蒸发过程中烟道内的气液分布和变化规律,喷嘴参数对蒸发性能的影响,以及蒸发过程随着负荷降低的变化规律。结果表明:液滴颗粒可在烟道内完全蒸发;粒径从40 μm增加到80 μm时,液滴蒸发时间从0.26 s增加到0.62 s,蒸发距离从6.15 m增加到13.41 m;蒸发时间和蒸发距离与液滴粒径近似呈线性关系;蒸发时间随着喷射角度的增加而减小;喷射角度为90°时,蒸发距离最短;喷射角度为120°时,蒸发距离最大;3种喷射方向中,逆流喷射方式蒸发时间最长,但蒸发距离最短;负荷降低,蒸发时间增加;负荷由75%降低至50%时,蒸发距离有显著提升。     

消油剂使用对水下溢油分散效果的研究

消油剂的水下使用是水下溢油应急处置的一种潜在的有效手段,但是消油剂对水下溢油分散效果的定量评估还比较少见。本研究采用自制的1 m×1 m×2 m（长×宽×高）的水下溢油模拟实验装置,开展消油剂作用下的蓬莱19-3原油水下喷射实验,以油滴体积分布和体积中值粒径为指标,考察不同消油剂使用量对水下溢油油滴破碎的影响。结果表明,与不使用消油剂相比,使用消油剂时的水下溢油分散效果更加显著,表现为油滴体积分布最高点向小粒径方向移动,大粒径油滴的体积分数减小;消油剂使用量越大,大粒径油滴的体积分数越小,最终完全消失。油滴体积中值粒径也随消油剂使用量的增加逐渐减小。     

南京一次典型雾霾天气气溶胶光学特性

利用太阳光度计测得的直射太阳辐射和天空扫描数据,对南京北郊2010年冬季一次雾霾天气过程中气溶胶的光学特性进行了反演研究.研究表明,雾霾影响期间气溶胶光学厚度(AOD)明显增加,在1020,870,675,440nm四个波段上,雾霾前AOD为0.16~0.43,雾霾影响期间为0.31~0.84,雾霾后为0.19~0.48;本次雾霾天气的局地气溶胶散射能力增强,单次散射反照率(SSA)由发生前的0.8~0.86增大到发生时的0.89~0.91,而复折射指数的虚部降低,气溶胶的吸收能力明显减弱;雾霾过程伴随了大尺度气溶胶的导入,同时也有人为排放的贡献.其中雾霾影响期间粗粒子模态的体积浓度是发生前的2.5倍,细粒子浓度也比发生前增长了90%.