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1.
An experimental and theoretical study has been carried out to investigate the rate of desorption of SO2 from water drops falling at terminal velocity in air. The experiments were carried out in the Mainz vertical wind tunnel in which water drops of various sizes containing S(IV) in various concentrations were freely suspended in the vertical airstream of the tunnel. The results of these experiments were compared with the predictions of three theoretical models, and with the experiments of Walceket al. This comparison shows that the predictions of the diffusion model of Kronig and Brink in the formulation given by Walcek and Pruppacher agree well with the experimental results for all relevant large and small rain-drop sizes, and for all considered concentrations of S(IV) inside the drops. In contrast, the predictions of the diffusion model which assumes complete internal mixing inside a drop agrees with the experimental results only if the concentration of S(IV) inside the drop is less than that equivalent of an equilibrium SO2 concentration of 15 ppbv. At larger concentrations, the theoretical predictions of the model for complete internal mixing progressively deviate from the experimental results. It is further shown that Barrie's double film model can be used to interpret the resistance to diffusion inside a drop in terms of a diffusion boundary layer inside the drop which increases in thickness with decreasing concentration of S(IV). Applying our results to the desorption of SO2 from small and large rain drops falling below an assumed cloud base, shows that for typical contents of S(IV) inside the drops substantial amounts of SO2 will desorb from these drops unless H2O2 is present in the surrounding air.  相似文献   

2.
An experimental investigation of the simultaneous absorption of NH3 and SO2 from the ambient atmosphere by freely falling water drops has been carried out in the Mainz vertical wind tunnel. The experimental results were found to be in good agreement with the results derived from computations with the Kronig-Brink convective diffusion model and also with a model which assumes a drop to be well mixed at all times. Encouraged by this agreement, these computation schemes for the uptake of gas by single drops where incorporated in a pollution washout model with realistic SO2, NH3 and CO2 gas profiles. This model allows an entire raindrop size distribution to fall through a gas layer. The results of this plume-model show that the SO2 uptake is strongly dependent on the NH3 concentration in the atmosphere and on the rainrate. We also find that the small drops contribute more towards the washout of these gases. In the case of simultaneous presence of NH3 and SO2, desorption of these gases is negligible.  相似文献   

3.
For the purpose of testing our previously described theory of SO2 scavenging a laboratory investigation was carried out in the UCLA 33 m long rainshaft. Drops with radii between 250 and 2500 m were allowed to come to terminal velocity, after which they passed through a chamber of variable length filled with various SO2 concentrations in air. After falling through a gas separating chamber consisting of a fluorocarbon gas the drops were collected and analyzed for their total S content in order to determine the rate of SO 2 absorption.The SO2 concentration in air studied ranged between 1 and 60% (v). Such relatively large concentrations were necessary due to the short times the drops were exposed to SO2 in the present setup. The present experimental results were therefore not used to simulate atmospheric conditions but rather to test our previously derived theory which is applicable to any laboratory or atmospheric condition. Comparison of our studies with the results from our theory applied to our laboratory conditions led to predicted values for the S concentration in the drops which agreed well with those observed if the drops had radii smaller than 500 m. In order to obtain agreement between predicted and observed S concentrations in larger drops, an empirically derived eddy diffusivity for SO2 in water had to be included in the theory to take into account the effect of turbulent mixing inside such large drops.In a subsequent set of experiments, drops initially saturated with S (IV) were allowed to fall through S-free air to determine the rate of SO 2 desorption. The results of these studies also agreed well with the results of our theoretical model, thus justifying the reversibility assumption made in our theoretical models.In a final set of experiments, the effects of oxidation on SO2 absorption was studied by means of drops containing various amounts of H2O2. For comparable exposure times to SO2, the S concentration in drops with H2O2 was found to be up to 10 times higher than the concentration in drops in which no oxidation occurred.  相似文献   

4.
A model with spectral microphysics was developed to describe the scavenging of nitrate aerosol particles and HNO3 gas. This model was incorporated into the dynamic framework of an entraining air parcel model with which we computed the uptake of nitrate by cloud drops whose size distribution changes with time because of condensation, collision-coalescence and break-up. Significant differences were found between the scavenging behavior of nitrate and our former results on the scavenging behavior of sulfate. These reflect the following chemical and microphysical differences between the two systems:
  1. nitrate particles occur in a larger size range than sulfate particles.
  2. HNO3 has a much greater solubility than SO2 and is taken up irreversibly inside the drops in contrast to SO2.
  3. nitric acid in the cloud water is formed directly on uptake of HNO3 gas whereas on uptake of SO2 sulfuric acid is formed only after the reaction with oxidizing agents such as e.g., H2O2 or O3.
  4. nitrate resulting from uptake of HNO3 is confined mainly to small drops, whereas sulfate resulting from uptake of SO2 is most concentrated in the largest, oldest drops, which have had the greatest time for reaction.
Sensitivity studies showed that the nitrate concentration of small drops is significantly affected by the mass accommodation coefficient.  相似文献   

5.
Differences in total iron and manganese concentrations between large (d > 23 m) and small (4 < d < 23 m) cloud and fog drops were investigated at four locations in the United States. The study examined coastal stratus and stratocumulus clouds in southern California and northern Oregon, frontal and orographic clouds at Mt. Mitchell, North Carolina, and radiation fogs in California's San Joaquin Valley. The speciation of iron as a function of drop size was also examined in some fog samples from the San Joaquin Valley. Total iron and manganese concentrations were generally higher in large drops than in small drops in clouds sampled at Mt. Mitchell and along the southern California coast. These species were typically enriched in small drops at the Oregon coast and San Joaquin Valley sites. Ratios of dissolved Fe(III) to total dissolved Fe ranged from 0.88 to 0.93 in small fog drops. Non-uniform distributions of iron and manganese across the drop size spectrum can influence rates of metal catalyzed S(IV) autooxidation. Approximately 50% of the sampled clouds were calculated to experience autooxidation rate enhancements greater than 30% due to variations in drop acidity and catalyst concentrations with drop size.  相似文献   

6.
An experimental study has been carried out in the Mainz vertical wind tunnel to determine the rate at which NH3 in the presence of CO2 is absorbed by freely suspended water drops. The experimental uptake rates were found to be in good agreement with the rates predicted by the Kronig-Brink convective diffusion model and, for gas concentrations in the ppbv range also by the model in which it is assumed that the absorbed gas is well mixed inside the drop (henceforth called well mixed model). The same conclusion was shown to apply also to the desorption of NH3 from a drop previously exposed to NH3. The latter result is in contrast to the desorption of SO2 which must be described by a model which accounts for the diffusion of the species inside the drop. Comparison of our experimental results with theory show further that the uptake of NH3 in presence of CO2 is significantly overestimated if the slow reaction CO2(aq)+H2OHCO 3 – +H+ is neglected in the theoretical computation.  相似文献   

7.
This paper deals with direct calculations of the radiation-equilibrium temperature profile in the Earth’s atmosphere from experimental spectroscopic data. The calculations are made for its present composition and for the modified ones, when concentration of a gas, namely, one of carbon dioxide CO2, methane CH4, nitrous oxide N2O or water vapor H2O is changed. Calculations were carried out with one-dimensional (horizontally homogeneous) radiation model proceeding from the values of absorption coefficients of atmospheric layers estimated from actual data. Calculations are carried out for small disturbances of the said gases’concentrations. Approximate estimates of large disturbance were made for the cases of total withdrawal of concrete gas from the atmosphere or, on the contrary, of large increase in its concentration.  相似文献   

8.
An experimental study involving the Mainz vertical wind tunnel is described where the rate of SO2 removed from the air by freely suspended water drops was measured for SO2 concentrations in the gas phase ranging between 50 and 500 ppb, and for various H2O2 concentrations in the liquid phase. In a first set of experiments, the pH inside the SO2 absorbing drops was monitored by means of colour pH indicators added to the drops. In a second set of experiments, the amount of SO2 scavenged by the drops was determined as sulfate by an ionchromatograph after the drops had been removed from the vertical air stream of the wind tunnel after various times of exposure to SO2. The results of our experimental study were compared with the theoretical gas diffusion model of Walcek and Pruppacher which was reformulated for the case of SO2 concentrations in the ppbv(v) range for which the main resistance to diffusion lies in the gas phase surrounding the drop. Excellent agreement between experiment and theory was obtained. Encouraged by this agreement, the theory was used to investigate the rate of sulfate production inside a drop as a function of pH. The sulfate production rate, which includes transport and oxidation, was compared with the production rate based on bulk equilibrium, as cited in the literature.  相似文献   

9.
An extention of our previous theory for trace gas absorption into freely-falling cloud and raindrops is presented. This theory describes the convective diffusion of a trace gas through air and into a water drop with internal circulation, the drop falling at its terminal velocity. Using flow fields for the circulating water inside and for the moving air outside the drop, obtained by numerical solutions to the Navier—Stokes equation of motion, we numerically solved the convective diffusion equation to determine the uptake of SO2 by water drops of various sizes, time exposure to the gas phase, and concentration of SO2 in the gas phase. It was found that for drops of radius larger than 1 mm and relatively low gas concentrations (10 ppb (v)), resistance to gas diffusion lies mainly in the gas phase; while for drops of radius less than 500 m and gas concentrations larger than those found in the atmosphere (1% (v)), the resistance to diffusion lies primarily in the liquid phase. With drop sizes and gas concentrations between these limits, the rate of SO2 uptake is controlled by a coupled resistance to diffusion inside and outside the drop. In addition to our general model, a simplified version was formulated which allows considerable savings in computer time for evaluation and improved ease of handling without significant loss of accuracy. A comparison between our simplified model and that of Barrie (1978) shows that the boundary-layer approach of Barrie may be a useful alternate approach to estimating trace gas absorption by water drops, provided appropriate values are chosen for the thickness of the boundary layers involved.  相似文献   

10.
In laboratory experiments the interactions of ammonia with ice crystals were studied within the temperature range between 0 and −20°C. In a first series of experiments dendritic ice crystals were grown from water vapor in presence of ammonia gas in various concentrations between 4 and 400 ppbv. In a second series of experiments pure ice crystals were exposed to a humidified ammonia–air mixture inside a horizontal flow tube. The influence of temperature, ammonia gas concentration (0.6, 1.5, and 10 ppmv), exposure time, and the presence of impurities such as sulfate on the ammonia uptake by the ice surface was investigated by determining the ammonium content in the melt water of the ice crystals by ion chromatography. During the growth of ice crystals significant amounts of ammonia (around 200 μg/l) were taken up even at small gas concentrations. In contrast, even at high gas concentrations the uptake of ammonia by non-growing ice crystals was lower by approximately one order of magnitude. The presence of sulfate on the ice surface affected an enhanced uptake of ammonia by a factor of 5–10. A model is presented which describes the uptake of ammonia by ice considering the chemical processes occurring in the ice surface layer and simultaneous diffusion of ammonia into bulk ice. Even the increased uptake of ammonia by growing ice is rather small compared to the uptake by water droplets; thus, the major process for scavenging of ammonia from the atmosphere via the ice phase might not be the direct uptake by ice crystals but the riming involving super-cooled droplets containing ammonia.  相似文献   

11.
Our previously developed theoretical models for describing the rate at which water-soluble atmospheric trace gases are scavenged by cloud and rindrops were evaluated for the case of acetaldehyde being absorbed and desorbed by water drops of radii between 250 to 2500 m radius. The experimental verification of our theoretical predictions was carried out in the UCLA 33 m high precipitation shaft in which falling water drops were allowed to come to terminal velocity before passing through a chamber of variable lengths filled with air containing acetaldehyde at various partial pressures. For all drop sizes studied, the experimental results and the theoretical predictions were in reasonable agreement.  相似文献   

12.
Cores of high radar reflectivity (>50 dBZ) and raindrops larger than 4 mm in diameter were occasionally reported in warm clouds, offshore from Hawaii. A kinematic numerical model with detailed microphysics was used to study the formation of these cores and the development of the giant drops. The role of collisional and spontaneous breakup of drops was evaluated. Our results show that spontaneous breakup of raindrops restricts the formation of giant drops (D>4 mm). This could be a result of the poor parameterization of the fragment size distribution, and the probabilities of the spontaneous breakup. The inclusion of only binary breakup mechanism explained the observed radar echoes and the drop spectra. These results corroborate the hypothesis that the updrafts in the Hawaiian clouds sort out different size drops in such a way that millimeter size drops are allowed to fall in an environment deficient of smaller raindrops. In this way, the large raindrops continue to grow by collection of small cloud droplets, but have a smaller chance for collisional breakup (the efficiency for this type of breakup is small for collisions with cloud droplets). The collisional breakup of big raindrops was also found to play a significant role in the formation of giant drops. Such drops are formed following collision–breakup of large raindrops in which one of the fragments is larger than the original drops.  相似文献   

13.
An experimental study of the scavenging of dichloromethane vapor by water drops falling at terminal velocity, has been carried out in the UCLA precipitation shaft, in order to test the predictions of theoretical washout models. Whereas good agreement between theory and experiment was found for drops of radius 0.332 mm, computed gas uptake rates for 1.253 and 2.21 mm radius drops were much slower than those measured, just as reported previously for the washout of both sulfur dioxide and acetaldehyde. An analysis shows that theory can be reconciled with all of the experimental data by replacing the compound specific aqueous phase Fickian molecular diffusion coefficient used in the theory, by an effective diffusivity, having a constant value, (3×10-4 cm2 s-1), independent of the physical and chemical nature of the absorbed species, for all drops of equivalent radii greater than 0.9 mm.  相似文献   

14.
Reliable cloud microphysical measurements can lead to a better understanding of the development of precipitation and cloud radiation. However, imaging of cloud particles with sizes < 200 μm has been limited to small (collected) samples of high-quality photographs or large quantities of poor-quality digital images. Here we introduce two new instruments with demonstrated abilities for improved measurements of cloud drop spectra, liquid water content and digital imaging of the size and shape of small ice crystals. The first instrument uses digital holography to increase the sample volume over that possible with in-focus imaging of small particles. The digital holograms can be processed automatically and are expected to reveal the size and shape of small ice crystals, and the three-dimensional concentration, spacing and liquid water content of cloud drops. The second instrument measures cloud drop spectra and liquid water content from high-resolution measurements of forward-scattered light from an ensemble of drops. This eliminates inherent problems of coincidence and the small sample volume associated with single-drop measurements of drops. The theory of measurement and results from tests of both instruments are presented.  相似文献   

15.
水滴冻结实验测量降水物中的冻结核含量   总被引：3，自引：1，他引：3  
文中介绍了一套新研制的均匀水滴冻结实验装置 ,实验水滴与周围环境同步冷却 ,其温度梯度很小 ,可控制降温速率 ,并能自动记录冻结事件 ,从而提高了实验的精度。用此装置对北京地区 1995年底至 1998年出现的各类降水样品进行了实验 ,由水滴冻结温度谱推算了降水的冻结核浓度 温度谱 ,并对结果进行了分析和讨论  相似文献   

16.
The reaction kinetics of S(IV) autoxidation catalyzed by single metal ions of Mn(II) and Fe(II) or Fe(III) and by a mixture of Mn(II) and Fe(II) under the conditions representative for acidified atmospheric liquid water was investigated. A simple power law kinetic model based on the stability constants for metal-sulfito complexes formed during the first step of a radical chain mechanism predicts well the kinetics for the reactions catalyzed by single metal ions. The calculated stability constants for iron (5.7×103 dm3 mol–1) and manganese (10×104 dm3 mol–1) sulfito complexes are close to those reported in the literature. The catalytic synergism between Mn(II) and Fe(II) was confirmed. For this system the following power law rate equation was suggested:rtot = SFe · rFe + SMn · rMn ,where rFe and rMn are the reaction rates in the presence of Fe(II) and Mn(II), respectively. SFe and SMn are proportional factors, which account for the synergistic effect. The proposed power law rate equation predicts the reaction kinetics very well. The values of SFe (1.35) and SMn (15) indicate that the influence of Fe(II)/Fe(III) on Mn(II)/Mn(III) cycling is larger than, vice versa, agreeing with the reaction mechanism proposed for the S(IV) autoxidation catalyzed by mixed metal ions.  相似文献   

17.
登陆台风麦德姆不同部位降水强度及谱特征   总被引：1，自引：1，他引：0       下载免费PDF全文
利用架设在福建省尤溪站和屏南站的两台PARSIVEL第2代激光雨滴谱仪对2014年7月23—25日影响福建省的台风麦德姆 (1410) 进行观测,尤溪站位于移动路径中轴,屏南站位于台风强降水的区域即右侧云系,观测显示了台风不同部位雨滴谱特征:台风麦德姆在外围右前侧和后侧以及残留云系出现强降水,台风中心为连续性降水,雨强变化平稳;台风右侧云系雨滴平均谱谱宽由宽变窄,小滴数浓度先增后减,大滴逐渐减少,移动路径中轴后侧的残留云系出现大滴数浓度和谱宽的突增;含水量与雨强变化一致, 雨强小于10 mm·h-1时,以大量的小粒子贡献为主,形状因子μ及斜率参数λ分布较广;雨强大于10 mm·h-1时,大滴的贡献随雨强增大而增大,μ及λ均减小;同时,可利用μ与λ线性函数关系对Gamma分布进行简化。  相似文献   

18.
不同降水强度对PM2.5的清除作用及影响因素   总被引：1，自引：0，他引：1       下载免费PDF全文
云和降水过程是大气污染物的重要清除途径,但由于降水过程和大气污染颗粒物本身的复杂性,目前降水过程对大气污染物的清除机制及影响因素有待深入研究。该文利用2014年3月—2016年7月在北京地区连续观测的PM2.5和降水数据,研究了不同降水强度对PM2.5的清除率,以及雨滴谱、风速和降水持续时间对PM2.5清除率的影响。研究表明:降水强度越大,对PM2.5清除效率越高。小雨、中雨和大雨对PM2.5清除率平均值分别为5.1%,38.5%和50.6%。小雨不但对PM2.5的清除率最低,而且对PM2.5的清除效果也存在很大差异,约50%的小雨个例中PM2.5质量浓度出现减小情况,而另外50%的小雨个例中,PM2.5质量浓度出现增加情况。在持续时间长或地面风速增大的情况下,小雨也表现出较高的清除率。在中雨和大雨情况下,PM2.5质量浓度均出现明显减小情况。但降水持续时间和风速对中雨和大雨的清除率影响较小,这是由于中雨和大雨一般在较短时间内即可清除大部分PM2.5,因此,对降水的持续时间和风速大小不敏感。  相似文献   

19.
Our previously described absorption model for the scavenging of trace gases by individual cloud and rain drops was applied to an ensemble of drops of given size distribution as found in typical atmospheric rainfalls. This study allowed: (1) determination of the redistribution which a pollution plume suffers as rain falls through it, and (2) determination of the amount of pollutant contained in. the fallen rain. For the present application it was assumed that the pollution plume consisted of SO2, only, and that its concentration varied vertically as a Gaussian distribution centered 200 m above the ground. Rain of various intensities and corresponding drop size distributions was allowed to pass through this pollution layer. The results of our study show that the average height and concentration of the plume decrease in proportion to the total amount of rain which had passed through the pollution layer. The fractional plume washout rate (in % per mm of rain) was found to be inversely proportional to the SO2 gas concentration, the plume height, and the plume thickness. By including the effects of oxidation inside the falling raindrops, it was noted that the removal of SO2 became enhanced by a factor of up to 10 times. For significant oxidation the rate with which SO2 was washed out was found to be inversely proportional to the rainfall rate. For the case of light drizzle (2 mm h-1) and large oxidation rate constants (100 s-1), as much as 40% of the sulfur load could be removed by 1 mm of rain. For the case of a heavier rainfall (25 mm h-1) composed of correspondingly larger drops, the washout rate varied between 2 and 10$ mm-1 over a wide range of oxidation rates.  相似文献   

20.
陈良吕  夏宇  庄潇然 《气象科技》2020,48(5):664-674
基于重庆市气象局中尺度数值预报业务系统,开展不同地形平滑方案对模式降水预报的影响研究,详细对比WRF模式中不使用地形平滑方案以及使用s-d-s和1-2-1两种平滑方案生成的静态地形高度场的差异,开展不同地形平滑方案批量平行试验并选取典型强降水个例进行对比分析,结果表明:不同地形平滑方案生成的静态地形高度场之间有明显的差异,特别是在地形较为陡峭的高原和山脉等地区,最大绝对偏差可达462.56m;s-d-s和1-2-1两种地形平滑方案主要平滑掉了模式地形中较小尺度的地形特征,且总体而言1-2-1方案的平滑效果比s-d-s方案明显。连续一个月批量平行试验降水预报检验结果表明,进行模式地形平滑对大雨及以上量级降水预报有正面影响,且使用1-2-1平滑方案的预报结果优于使用s-d-s平滑方案的预报结果;降水个例对比分析结果表明:采用不同的地形平滑方案会造成垂直速度和水汽通量散度预报的明显差异,这样的明显差异会进而影响强降水预报的落区和强度。  相似文献   

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