The Vertical Transport of Air Pollutants by Convective Clouds. Part I: A Non-Reactive Cloud Transport Model   总被引：1，自引：0，他引：1  

Kong Fanyou  Qin Yu 《大气科学进展》1993,10(4):415-427

A convective cloud transport model, without chemical processes, is developed by joining a set of concentration conservative equations into a two-dimensional, slab-symmetric and fully elastic numerical cloud model, and a numerical experiment is completed to simulate the vertical transport of ground-borne, inert gaseous pollutant by deepthunderstorm. The simulation shows that deep convective storm can very effectively transport high concentrated pollutant gas from PBL upward to the upper troposphere in 30 to 40 minutes, where the pollutant spreads laterally outward with strong anvil outflow, forming an extensive high concentration area. Meanwhile, relatively low concentration areas are formed in PBL both below and beside the cloud, mainly caused by dynamic pumping effect and sub-cloud downdraft flow. About 80% of the pollutant gas transported to the upper troposphere is from the layer below 1.5 km AGL (above ground level).  相似文献   

Phase partitioning of aerosol particles in clouds at Kleiner Feldberg     

A. Hallberg  K. J. Noone  J. A. Ogren  I. B. Svenningsson  A. Flossmann  A. Wiedensohler  H. -C. Hansson  J. Heintzenberg  T. L. Anderson  B. G. Arends  R. Maser 《Journal of Atmospheric Chemistry》1994,19(1-2):107-127

The partitioning of aerosol particles between cloud droplets and interstitial air by number and volume was determined both in terms of an integral value and as a function of size for clouds on Mt. Kleiner Feldberg (825 m asl), in the Taunus Mountains north-west of Frankfurt am Main, Germany. Differences in the integral values and the size dependent partitioning between two periods during the campaign were observed. Higher number and volume concentrations of aerosol particles in the accumulation mode were observed during Period II compared to Period I. In Period I on average 87±11% (±one standard deviation) and 73±7% of the accumulation mode volume and number were incorporated into cloud droplets. For Period II the corresponding fractions were 42±6% and 12±2% in one cloud event and 64±4% and 18±2% in another cloud event. The size dependent partitioning as a function of time was studied in Period II and found to have little variation. The major processes influencing the partitioning were found to be nucleation scavenging and entrainment.  相似文献   

Computer modelling of clouds at Kleiner Feldberg     

R. N. Colvile  R. Sander  T. W. Choularton  K. N. Bower  D. W. F. Inglis  W. Wobrock  D. Schell  I. B. Svenningsson  A. Wiedensohler  H. -C. Hansson  A. Hallberg  J. A. Ogren  K. J. Noone  M. C. Facchini  S. Fuzzi  G. Orsi  B. G. Arends  W. Winiwarter  T. Schneider  A. Berner 《Journal of Atmospheric Chemistry》1994,19(1-2):189-229

The airflow, cloud microphysics and gas- and aqueous-phase chemistry on Kleiner Feldberg have been modelled for the case study of the evening of 1 November 1990, in order to calculate parameters that are not easily measured in the cloud and thus to aid the interpretation of the GCE experimental data-set. An airflow model has been used to produce the updraught over complex terrain for the cloud model, with some care required to ensure realistic modelling of the strong stable stratification of the atmosphere. An extensive set of measurements has been made self-consistent and used to calculate gas and aerosol input parameters for the model. A typical run of the cloud model has calculated a peak supersaturation of 0.55% which occurs about 20 s after entering cloud where the updraught is 0.6 m s^–1. This figure has been used to calculate the efficiency with which aerosol particles were scavenged; it is higher than that calculated by other methods, and produces a cloud with slightly too many droplets. A broad cloud droplet size spectrum has been produced by varying the model inputs to simulate turbulent mixing and fluctuations in cloud parameters in space and time, and the ability of mixing processes near cloud-base to produce a lower peak supersaturation is discussed. The scavenging of soluble gases by cloud droplets has been observed and departures from Henry's Law in bulk cloud-water samples seen to be caused by variation of pH across the droplet spectrum and the inability of diffusion to adjust initial distributions of highly soluble substances across the spectrum in the time available. Aqueous-phase chemistry has been found to play a minor role in the cloud as modelled, but circumstances in which these processes would be more important are identified.  相似文献   

The vertical transport of air pollutants by convective clouds Part II: Transport of soluble gases and sensitivity tests     

Kong Fanyou 《大气科学进展》1994,11(1):1-12

A two-dimensional, non-reactive convective cloud transport model is used to simulate in detail the vertical transport and wet scavenging of soluble pollutant gases by a deep thunderstorm system, Simulations show that for gases with not very high solubility, a deep and intense thunderstorm can still rapidly and efficiently transport them from boundary layer (PBL) up to mid and upper troposphere, resulting in a local significant increase of concentration in the upper layer and a reduction in PBL. Dissolution effects decrease both the incloud gas concentration and the upward net fluxes. The higher the solubility is, the more remarkable the decrease is. However, for very low soluble gases (H < 102 M atm-1), the influences are very slight. In addition, the effects of irreversible dissolution and aqueous reactions in drops on the vertical transport of gaseous pollutants are estimated in extreme.  相似文献   

气溶胶核化清除的化学效应 I：云滴化学非均匀性的研究     

刘小红  洪钟祥  王明康 《大气科学》1994,18(4):385-395

本文将水汽在云滴上凝结增长的物理过程与气溶胶、气体的化学过程相结合，对气溶胶核化清除的化学效应进行了研究。 计算结果表明:气溶胶的核化清除造成了云滴化学成分随云滴大小分布的非均匀性，这种非均匀性又对云滴内发生的气体吸收、液相氧化产生影响。 本文还比较了不同污染状况下，不同大小的云滴内气溶胶核化清除与液相氧化对云滴化学的相对贡献的差异。 因此，这种云滴化学的非均匀性(云微化学)的研究对于云化学的野外观测及数值模拟都是重要的。  相似文献   

Natural radionuclides in the Arabian Sea and Bay of Bengal: Distribution and evaluation of particle scavenging processes     

M. M. Sarin  R. Rengarajan  B. L. K. Somayajulu 《Journal of Earth System Science》1994,103(2):211-235

Vertical and temporal variations in the activities of²³⁴Th,²¹⁰Po and²¹⁰Pb have been measured, in both dissolved and paniculate phases, at several stations in the eastern Arabian Sea and north-central Bay of Bengal. A comparative study allows us to make inferences about the particle associated scavenging processes in these two seas having distinct biogeochemical properties. A common feature of the²³⁴Th profiles, in the Arabian Sea and Bay of Bengal, is that the dissolved as well as total (dissolved + particulate) activity of²³⁴Th is deficient in the surface 200 m with respect to its parent,²³⁸U. This gross deficiency is attributed to the preferential removal of²³⁴Th by adsorption onto settling particles which account for its net loss from the surface waters. The scavenging rates of dissolved²³⁴Th are comparable in these two basins. The temporal variations in the²³⁴Th-²³⁸U disequilibrium are significantly pronounced both in the Arabian Sea and Bay of Bengal indicating that the scavenging rates are more influenced by the increased abundance of particles rather than their chemical make-up. In the mixed layer (0–50 m), the scavenging residence time of²³⁴Th ranges from 30 to 100 days. The surface and deep waters of both the seas show an enhanced deficiency of dissolved²¹⁰Po relative to²¹⁰Pb and that of²¹⁰Pb relative to²²⁶Ra. The deficiencies of both²¹⁰Po and²¹⁰Pb in the dissolved phases are not balanced by their abundance in the particulate form indicating a net loss of both these nuclides from the water column. The scavenging rates of²¹⁰Po and²¹⁰Pb are significantly enhanced in the Bay of Bengal compared to those in the Arabian Sea. The mean dissolved²¹⁰Po/²¹⁰Pb and²¹⁰Pb/²²⁶Ra activity ratios in deep waters of the Bay of Bengal are ∼ 0.7 and 0.1, respectively, representing some of the most pronounced disequilibria observed to date in the deep sea. The Bay of Bengal and the Arabian Sea appear to be the regions of most intense particle moderated scavenging processes in the world oceans. This is evidenced by the gross disequilibria exhibited by the three isotope pairs used in this study.  相似文献   

On the scavenging of SO2 by cloud and raindrops: I. A theoretical study of SO2 absorption and desorption for water drops in air     

C. J. Walcek  H. R. Pruppacher 《Journal of Atmospheric Chemistry》1983,1(3):269-289

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   

Disequilibria between ²¹⁰Po and ²¹⁰Pb in surface waters of the southern South China Sea and their implications   总被引：1，自引：0，他引：1  

Yang Weifeng  Huang Yipu  Chen Min  Zhang Lei  Li Hongbin  Liu Guangshan  Qiu Yusheng 《中国科学D辑(英文版)》2006,49(1):103-112

Activities of the naturally occurring radionuclides, ²¹⁰Pb and ²¹⁰Po, were measured in both dissolved (<0.45 μm) and particulate (>0.45 μm) phases from surface waters of the southern South China Sea. The average activity of particulate ²¹⁰Pb, 0.23 Bq/m³ (n=23), accounted for about 12% of the total ²¹⁰Pb, which corresponds with values of open oceans. Particulate ²¹⁰Po, with an average activity of 0.43 Bq/m³, accounted for about 40% of the total ²¹⁰Po, which was much higher than those of open and eutrophic oceans. The residence times of total ²¹⁰Po and ²¹⁰Pb in surface waters estimated from an irreversible steady-state model were 0.82 a and 1.16 a, respectively. The consistently high fractionation factor calculated either by scavenging rate constants (5.42) or K_d values (6.69) suggested that a significant fractionation occurred between ²¹⁰Po and ²¹⁰Pb during their removal from solution to particles and that the two radionuclides had different biogeochemical cycling pathways in the oligotrophic South China Sea. Furthermore, our results indicated that there exist different fractionation mechanisms between ²¹⁰Po and ²¹⁰Pb in different marine environments: in eutrophic ocean, plankton detritus and fecal pellets are the main carrier of ²¹⁰Po and ²¹⁰Pb, by which ²¹⁰Po and ²¹⁰Pb have been scavenged and removed; while in oligotrophic ocean, microbes could become the main carrier of ²¹⁰Po and fractionate ²¹⁰Po and ²¹⁰Pb significantly as a result of scarce plankton detritus and fecal pellets. These results suggest the use of ²¹⁰Po to trace marine biogeochemical processes relating to microbial activities and the cycling of sulfur group elements (S, Se, Te and Po).  相似文献   

Numerical Investigation of Gas Scavenging by Weak Precipitation     

Leiming Zhang  Robert Vet  Diane V. Michelangeli 《Journal of Atmospheric Chemistry》2006,54(3):203-231

A one-dimensional cloud model with size-resolved microphysics and size-resolved aqueous-phase chemistry, driven by prescribed dynamics, has been used to study gas scavenging by weak precipitation developed from low-level, warm stratiform clouds. The dependence of the gas removal rate on the physical and chemical properties of precipitation has been explored under controlled initial conditions. It is found that the removal of four gaseous species (SO₂, NH₃, H₂O₂ and HNO₃) strongly depends on the total droplet surface area, regardless the mean size of droplets. The removal rates also correlate positively with the precipitation rate, especially for precipitation having a mean radius larger than 20 μm. The dependence of the scavenging coefficients on the total droplet surface area is stronger than on the precipitation rate. The removal rates of SO₂, NH₃ and H₂O₂ by precipitation strongly depend on the others' initial concentrations. When NH₃ (or H₂O₂) concentration is much lower than that of SO₂, the removal rate of SO₂ is then controlled by the concentration of H₂O₂ (or NH₃). The removal of NH₃ (or H₂O₂) also directly depends on the concentration of SO₂. NH₃ and H₂O₂ can also indirectly affect each other's removal rate through interaction with SO₂. The scavenging coefficient of SO₂ increases with the concentration ratio of NH₃ to SO₂ if the ratio is larger than 0.5, while the scavenging coefficient of NH₃ increases with the concentration ratio of SO₂ to NH₃ when the ratio is smaller than 1. The scavenging coefficient of H₂O₂ generally increases with the concentration ratio of SO₂ to H₂O₂. Although the Henry's law equilibrium approach seems to be able to simulate gas scavenging by cloud droplets, it causes large errors when used for simulating the scavenging of soluble gas species by droplets of precipitating sizes.  相似文献   

Rapid change in nitrate and sulfate concentrations observed in early stage of precipitation and their deposition processes     

Hiroaki Minoura  Yasunobu Iwasaka 《Journal of Atmospheric Chemistry》1996,24(1):39-55

The concentrations of H⁺, nitrate (NO₃ ^-), and sulfate (SO₄ ^2-) in rainwater and their temporal changes were analyzed on the basis of continuous observation from 1 July 1991 to 30 June 1992 at a suburb of Nagoya, Japan. The yearly average for pH was 4.4. In general, an increasing pH with increase in precipitation amount was observed for rain events. Relatively high pH rainwater was sometimes observed at the beginning of rainfall, even though high concentrations of NO₃ ^- and SO₄ ^2- were involved. The high pH values were considered to be caused by the neutralization process with particulate matter containing cations. The yearly averaged ratio of equivalent concentration of nitrate to sulfate (N/S) in rainwater was 0.58. In the early stage of rain, the N/S value was usually more than 1.0 due to the difference of scavenging process between NO₃ ^- and SO₄ ^2-. High values of N/S ranging from 5 to 10 were found under the atmospheric conditions of calm winds and low humidity, during which it is possible that atmospheric particles float for a long time in the air before a rain event. The adsorption of NO₃ ^- in the early stage of rainfall by particulate matter was suggested from the difference in scavenging processes of NO₃ ^- and SO₄ ^2-. A possible scavenging process, called limb cloud scavenging, is presented to explain the interaction of particles and nitrate ions at the early stage of rain. In limb cloud scavenging, the repeated migration of cloud particles or raindrops between the inside and outside of clouds increases the absorption of ions to a highly condensed level, thus increasing the N/S value of rainwater. The influence of global scale seasonal phenomena with large amounts of particulates, such as typhoons or Asian dust storms, was also studied.  相似文献