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1.
In November 1993 an airborne field study was performed in order to investigate the microphysical and radiative properties of cooling tower water clouds initiated by water vapour emissions and polluted by the exhaust from coal-fired power plants. The number-median diameter of the droplet size distributions of these artificial clouds was in the range of 13 μm. The concentration of smaller droplets (diameters dD < 10 μm) increased with height and horizontal distance from the cooling towers. Close to the cooling towers, bimodal spectra were found with a second mode at 19 μm. The liquid water content (LWC) ranged between 2 and 5 g/m3 and effective droplet radii (Re) between 6 and 9 μm were measured. LWC and Re decreased with altitude, whereas the droplet concentration (ND) remained approximately constant (about 2000 cm−3 ). An enrichment of interstitial aerosol particles with particle diameters (dp) smaller 0.2 μm compared to the power plant plume in the vicinity of the clouds was observed. Particle activation for dm > 0.3 μm. was evident, especially in cooling tower clouds further apart and separated from their sources. Furthermore, radiation measurements were performed, which revealed differences in the vertical profiles of downwelling solar and UV radiation flux densities inside the clouds.The effective droplet radius Re was parameterized in terms of LWC and ND using equations known from literature. The close agreement between measured and parameterized Re indicates a similar coupling of Re, LWC and ND as in natural clouds.By means of Mie calculations, volume scattering coefficients and asymmetry factors are derived for both the cloud droplets and the aerosol particles. For the cloud droplets, the optical parameters were described by parameterizations from the literature. The results show, that the link between radiative and microphysical properties of natural clouds is not changed by the extreme pollution of the artificial clouds.  相似文献   

2.
A global three-dimensional model of the tropospheric sulfur cycle   总被引:9,自引:0,他引:9  
The tropospheric part of the atmospheric sulfur cycle has been simulated in a global three-dimensional model. The model treats the emission, transport, chemistry, and removal processes for three sulfur components; DMS (dimethyl sulfide), SO2 and SO4 2– (sulfate). These processes are resolved using an Eulerian transport model, the MOGUNTIA model, with a horizontal resolution of 10° longitude by 10° latitude and with 10 layers in the vertical between the surface and 100 hPa. Advection takes place by climatological monthly mean winds. Transport processes occurring on smaller space and time scales are parameterized as eddy diffusion except for transport in deep convective clouds which is treated separately. The simulations are broadly consistent with observations of concentrations in air and precipitation in and over polluted regions in Europe and North America. Oxidation of DMS by OH radicals together with a global emission of 16 Tg DMS-S yr–1 from the oceans result in DMS concentrations consistent with observations in the marine boundary layer. The average turn-over times were estimated to be 3, 1.2–1.8, and 3.2–6.1 days for DMS, SO2, and SO4 2– respectively.  相似文献   

3.
By making use of TOVS Path-B satellite retrievals and ECMWF reanalyses, correlations between bulk microphysical properties of large-scale semi-transparent cirrus (visible optical thickness between 0.7 and 3.8) and thermodynamic and dynamic properties of the surrounding atmosphere have been studied on a global scale. These clouds constitute about half of all high clouds. The global averages (from 60°N to 60°S) of mean ice crystal diameter, De, and ice water path (IWP) of these clouds are 55 μm and 30 g m−2, respectively. IWP of these cirrus is slightly increasing with cloud-top temperature, whereas De of cold cirrus does not depend on this parameter. Correlations between De and IWp of large-scale cirrus seem to be different in the midlatitudes and in the tropics. However, we observe in general stronger correlations between De and IWP and atmospheric humidity and winds deduced from the ECMWF reanalyses: De and IWP increase both with increasing atmospheric water vapour. There is also a good distinction between different dynamical situations: In humid situations, IWP is on average about 10 gm−2 larger in regions with strong large-scale vertical updraft only that in regions with strong large-scale horizontal winds only, whereas the mean De of cold large-scale cirrus decreases by about 10 μm if both strong large-scale updraft and horizontal winds are present.  相似文献   

4.
A one-dimensional, time-dependent model of the physics and chemistry of a warm stratiform cloud is used to study the possible impact of chemical inhomogeneity among cloud and raindrops on the oxidation of SO2 in clouds. The effects of chemical inhomogeneity are examined using two contrasting models: In Model 1 a bulk-solution parameterization is adopted which effectively treats all cloud and raindrops as if they are chemically homogeneous; in Model 2 we allow the cloud and raindrops to have a dichotomous distribution. The dichotomous distribution in Model 2 is simulated by assuming that the two groups of cloud droplets nucleate from two chemically distinct populations of condensation nuclei; one being acidic and the other being alkaline. While the two models yield essentially identical results when the ambient levels of H2O2 are greater than the ambient levels of SO2, the rate of conversion of SO2 to sulfuric acid and the amount of sulfate removed in the precipitation can be significantly enhanced in Model 2 over that of Model 1 under conditions of oxidant limitation (i.e., H2O2 < SO2). This enhancement is critically dependent upon the fraction of alkaline nuclei assumed to be present in Model 2 and arises from the rapid increase in the aqueous-phase reaction between O3+SIV at high pH. Our results suggest that cloud models which adopt a bulk-solution parameterization for cloud droplet chemistry, may underestimate the amount of in-cloud SO2 oxidation under oxidant-limited conditions.  相似文献   

5.
The pK 1 * and pK 2 * of H2SO3 have been determined in NaCl solutions as a function of ionic strength (0.1 to 6 m) and temperature (5 and 25 °C). The extrapolated values in water were found to be in good agreement with literature data. The experimental results have been used to determine the Pitzer interaction parameters for SO2, HSO 3 - and SO 3 - in NaCl solutions. The resultant parameters for NaHSO3 and Na2SO3 were found to be in reasonable agreement with the values for NaHSO4 and Na2SO4. It, thus, seems reasonable to assume that the interactions of Mg2+ and Ca2+ with HSO 3 - and SO 3 - can be estimated from the values with HSO 4 - and SO 4 - until experimental values are available. Measurements of pK 1 * and pK 2 * in artificial seawater were found to be in good agreement with the calculated values using the derived Pitzer parameters. It is, thus, possible to make reasonable estimates of the activity coefficients of HSO 3 - and SO 3 - ions and pK 1 * and pK 2 * for the ionization of H2SO3 in marine aerosols.  相似文献   

6.
The rainout-removal of SO2 and the acidification of precipitation from stratiform clouds are simulated using a one-dimensional, time-dependent model, parameterized microphysically in which dissolution and dissociation of gaseous SO2 and H2O2, and oxidation reaction in aqueous phase are taken into account. The effects of dynamic factors, including updraft flow and turbulent transport, and the concentration of gaseous SO2 and H2O2 being transported into the clouds on pH value of the precipitation, the conversion rateS(IV)-S(VI) and the wet deposition rate of SO2 are discussed. This work was supported by fund from the National Scientific Foundation of China.  相似文献   

7.
In recent years, China has implemented several measures to improve air quality. The Beijing-Tianjin-Hebei(BTH)region is one area that has suffered from the most serious air pollution in China and has undergone huge changes in air quality in the past few years. How to scientifically assess these change processes remain the key issue in further improving the air quality over this region in the future. To evaluate the changes in major air pollutant emissions over this region, this paper employs ens...  相似文献   

8.
RMAPS_Chem V1.0系统是基于WRF_Chem模式建立的服务于华北区域雾霾等污染预报业务的模式系统,该研究着重针对系统中污染排放清单不确定性带来的SO2浓度预报偏差较大问题,采用EnKF源反演和误差统计订正相结合的方法对排放清单进行了改进,形成了一套优化后的华北区域SO2排放清单。通过输入初始清单和优化清单对2017年10月进行模拟,并与华北地区616个地面环境监测站观测值进行对比,结果表明:EnKF源反演结合误差统计订正的排放清单优化方法适用于SO2排放清单的改进,有效降低了清单系统性偏差,针对主要区域及重点城市的检验显示模拟结果接近观测值;排放清单优化后模拟误差显著降低,如河北南部、山东西部至北京一带模式预报均方根误差与归一化平均绝对误差明显下降,区域内站点模拟误差呈正态分布特征,误差分布范围、最大概率出现范围均明显变窄,且最大误差概率明显上升。  相似文献   

9.
The interaction of formaldehyde with SO2 dissolved in the aqueous phase of clouds leads to the formation of hydroxymethane sulfonate. The impact of this process upon the gas-liquid equilibrium distribution of SO2 in rain clouds and the ensuing wet SO2 precipitation rate is explored. Model vertical SO2 distributions are derived from observational data for three atmospheric regions: continental polluted, continental remote, and marine. The wet deposition rate for SO2 in the polluted atmosphere increases by about a factor of two in the presence of formaldehyde compared with its absence. The effect is much stronger in the remote atmosphere leading to a potentially significant enhancement of wet SO2 deposition. In the marine atmosphere, wet deposition of SO2 may contribute as much as 35% to the total removal rate for SO2 by all processes including dry deposition and chemical conversion to sulfate.  相似文献   

10.
Aerosol size distributions were measured with Micro Orifice Uniform Deposit Impactor (MOUDI) cascade impactors at the rural Angiola and urban Fresno Supersites in California's San Joaquin Valley during the California Regional PM10/PM2.5 Air Quality Study (CRPAQS) winter campaign from December 15, 2000 to February 3, 2001. PM2.5 filter samples were collected concurrently at both sites with Sequential Filter Samplers (SFS). MOUDI nitrate (NO3) concentrations reached 66 μg/m3 on January 6, 2001 during the 1000–1600 PST (GMT-8) period. Pair-wise comparisons between PM2.5 MOUDI and SFS concentrations revealed high correlations at the Angiola site (r > 0.93) but more variability (r < 0.85) at the Fresno site for NO3, sulfate (SO4=), and ammonium (NH4+). Correlations were higher at Fresno (r > 0.87) than at Angiola (r < 0.7) for organic carbon (OC), elemental carbon (EC), and total carbon (TC). NO3 and SO4= size distributions in Fresno were multi-modal and wider than the uni-modal distributions observed at Angiola. Geometric mean diameters (GMD) were smaller for OC and EC than for NO3 and SO4= at both sites. OC and EC were more concentrated on the lowest MOUDI stage (0.056 µm) at Angiola than at Fresno. The NO3 GMD increased from 0.97 to 1.02 µm as the NO3 concentration at Angiola increased from 43 to 66 µg m− 3 during a PM2.5 episode from January 4–7, 2001. There was a direct relationship between GMD and NO3 and SO4= concentrations at Angiola but no such relationships for OC or EC. This demonstrates that secondary aerosol formation increases both concentration and particle size for the rural California environment.  相似文献   

11.
应用大气化学模式WRF-Chem(Weather Research and Forecast-Chemistry),分别选用亚洲排放源清单INTEX-B(Intercontinental Chemical Transport Experiment-Phase B)、REASv2.1(Regional Emission inventory in Asia version 2.1)以及全球排放源清单HTAP_v2(Hemispheric Transport of Air Pollution version 2),对浙江省2013年12月进行模拟,分别记为IN、RE和HT试验,研究人为源排放清单对大气污染物浓度数值模拟的影响。结果表明,3组试验合理的反映出PM2.5(空气动力学当量直径小于等于2.5μm的颗粒物,即细颗粒物)、PM10(空气动力学当量直径小于等于10μm的颗粒物,即可吸入颗粒物)和NO_2近地面浓度的时空分布特征,相关系数为0.5~0.8,85%以上的模拟值落在观测值的0.5~2倍范围内,但对SO_2近地面浓度模拟较差。IN、RE、HT试验对PM2.5和PM10的模拟偏差均成递减趋势,约为30%、16%和6%,HT试验的模拟值更加接近观测。INTEX-B清单中PM2.5的一次排放与二次气溶胶前提物SO_2均高于REAS与HTAP清单,因此会导致更多的硫酸盐生成,从而进一步增加PM2.5浓度。HTAP_v2清单中较低的NH3排放会抑制硝酸盐的生成,从而有助于降低PM2.5浓度。3个清单的基准年与模拟年的差异对SO_2浓度模拟的准确性影响更大,INTEX-B清单中SO_2排放量明显高于REASv2.1与HTAP_v2清单,尤其在浙北和沿海工业发达地区,导致IN试验模拟的SO_2在这些地区存在明显高估。3组试验模拟的NO_2浓度偏差最小且更为接近(-8%~4%),主要原因是3个清单在浙江省的NOx排放十分一致。从3组试验结果之间的差异程度来看,浙江省范围内PM2.5、PM10、SO_2和NO_2逐日浓度模拟值之间的平均差异程度分别约为14%、15%、51%和16%,最大差异程度分别为69%、78%、137%和132%。月均浓度与逐日浓度的平均差异程度基本一致,但最大差异程度明显更低。总体来看3组试验模拟的PM2.5、PM10与NO_2的差异程度明显低于SO_2。  相似文献   

12.
Research flights in November 1990 over the central parts of the United States, Wyoming and Colorado, were aimed to the investigation of the properties and microstructure of cirrus clouds (mainly cirrocumulus lenticularis). Among the other parameters measured on board the NCAR Saberliner were the concentration and size distribution of submicron particles and, in some cases, the particle deliquescence. For coarse insoluble particles found inside and outside of cloud elements, size distributions and morphology information were obtained by evaluating inertial impactor samples with an optical microscope and scanning electron microscope. In addition, the coarse particle composition was determined by x-ray energy spectrum analysis. The following conclusions from these measurements are:The large and coarse particle size distribution can be roughly simulated by a log-normal function with the modus around r=0.5 μm. Particle concentrations are very variable between several tenths and several particles per cm3. Particle volume distribution features a distinct maximum around 0.75 μm without a broad plateau which was observed in the case of sampling at lower altitude. Aerosol composition heterogeneity at cirrus cloud level is well documented by the evaluation of the fine particle sampling taken with the UMR sampling system. This heterogeneity can be partly explained by the interaction between aerosol and cloud elements, which is documented by the measured particle size distribution curves inside and outside of cloud elements. Assuming that particle deliquescence is caused by H2SO4 and/or by (NH4)2SO4, particle soluble mass fractions were found to be around 30% in the first case and about 40% in the second. The most frequently occurring elements in large and coarse particles at cirrus cloud level were Si, Cl, Ba, S, Ca and C.  相似文献   

13.
以武汉市为研究区域,基于实地调查获得典型行业污染源活动水平,以大气污染物排放清单编制技术指南为参考,利用排放因子法建立2014年武汉市大气污染源排放清单,并结合经纬度、人口密度分布、土地利用类型、道路长度等数据将排放清单进行了3 km×3 km网格化处理.结果表明,2014年武汉市SO2、NOx、PM10、PM2.5、CO、BC、OC、VOCs和NH3排放量分别为10.3、17.0、16.3、7.1、63.1、0.6、0.4、19.8和1.6万t.固定燃烧源为SO2排放的主要来源,其贡献率约64%;移动源为NOx的主要来源,其贡献率约51%;颗粒物排放主要来源于扬尘源和工艺过程源;CO和VOCs主要来源于工艺过程源,BC和OC排放均以移动源和生物质燃烧源为主,NH3排放主要来自农业源.污染物排放主要集中在青山区至新洲区一带.  相似文献   

14.
The effect of clouds and cloud chemistry on tropospheric ozone chemistry is tested out in a two-dimensional channel model covering a latitudinal band from 30 to 60° N. Three different methods describing how clouds affect gaseous species are applied, and the results are compared. The three methods are:
  • ?A first order parameterization scheme for the removal of sulphur and other soluble gases by liquid droplets.
  • ?A parameterization scheme for SO2, O3, and H2O2 removal is constructed. The scheme is based on the solubility of gases in liquid droplets, cycling times of air masses between clouds and cloud free areas and on the chemical interaction of SO2 with H2O2 and O3 in the liquid phase.
  • ?Gas-aqueous-phase interactions and aqueous-phase chemical reactions are included in the reaction scheme for a number of components in areas where clouds are present.
  • In all three methods, a full gas-phase chemistry scheme is used. Particular emphasis is given to the study of how the ozone and hydrogen peroxide levels are affected. Significant changes in the distributions are found when aqueous-phase chemical reactions are included. The result is loss of ozone in the aqueous phase, with pronounced reductions in ozone levels in the middle and lower troposphere. Ozone levels are reduced by 10 to 30% with the largest reductions in the remote middle troposphere, bringing the values in better agreement with observations. Changes in H2O2 are harder to predict. Although, in one case study, hydrogen peroxide is produced within the aqueous phase, concentrations are mostly comparable or even lower than in the other cases. Hydrogen peroxide levels are, however, shown to be very pH sensitive. pH values around 5 seem to favour high H2O2 levels. High H2O2 concentrations may be found particularly in the upper part of the clouds under favourable conditions.  相似文献   

    15.
    《Climate Policy》2013,13(1):40-55
    Recognizing the potential for over- as well as under-estimating the mitigation costs of non-CO2 greenhouse gases in an offset programme, this article examines the accuracy of cost estimates prepared by government agencies for the control of other types of emissions from small/medium sources via an offset programme. Specifically, analogy is made to the control of SOx and NOx controlled by California's Regional Clean Air Incentives Market (RECLAIM) Program. Even allowing for the energy crisis in 2000–2001 that drove up NOx emissions and control costs, it appears that the engineering cost methods used turned out to be generally accurate, defined as ±25%. Although such a finding does not ensure that the same results will apply to the case of non-CO2 GHGs, it certainly reinforces the growing literature on ex ante—ex post cost comparisons of environmental controls.  相似文献   

    16.
    Substitution of natural gas for coal is one means of reducing carbon dioxide (CO2) emissions. However, natural gas and coal use also results in emissions of other radiatively active substances including methane (CH4), sulfur dioxide (SO2), a sulfate aerosolprecursor, and black carbon (BC) particles. Will switching from coal to gas reduce the net impact of fossil fuel use on global climate? Using the electric utility sector as an example, changes in emissions of CO2, CH4,SO2 and BC resulting from the replacement of coal by natural gas are evaluated, and their modeled net effect on global mean-annual temperature calculated. Coal-to-gas substitution initially produces higher temperatures relative to continued coal use. This warming is due to reduced SO2 emissionsand possible increases in CH4 emissions, and can last from 1 to 30years, depending on the sulfur controls assumed. This is followed by a net decrease in temperature relative to continued coal use, resulting from lower emissions of CO2 and BC. The length of this period and the extent of the warming or cooling expected from coal-to-gas substitution is found to depend on key uncertainties and characteristics of the substitutions, especially those related to: (1) SO2 emissions and consequentsulphate aerosol forcing; and (2) the relative efficiencies of the power plantsinvolved in the switch.  相似文献   

    17.
    对非球形冰晶94 GHz云雷达后向散射和衰减的研究   总被引:1,自引:0,他引:1  
    针对94 GHz毫米波云雷达的数据处理,基于离散偶极子近似法(DDA)计算了几种非球形冰晶的后向散射及衰减效率,探讨了不同冰云模型下冰云的雷达反射率因子(Z_e)和衰减系数(k)及冰水含量(IWC,记作W)的关系。结果表明:(1)形状对冰晶的散射及衰减效率与粒子大小有关。(2)在实际的冰云中,将六角形冰晶和椭圆冰晶看做同体积的球形粒子将低估其衰减和后向散射。将聚合物冰晶看做等体积球形,将高估其后向散射及衰减,子弹花冰晶的后向散射与同体积的球形相比有减小也有增大,但是衰减比同体积球形的小。(3)冰云模型对Z_e-k、Z_e-W关系具有较大影响,假设滴谱相同的条件下,得到了具体冰云模型下对应Z_e-k、Z_e-W关系的系数。这些探讨为我国W波段云雷达的数据处理提供了参考。  相似文献   

    18.
    A Forest SO2 Absorption Model (ForSAM) was developed to simulate (1) SO2 plume dispersion from an emission source, (2) subsequent SO2 absorption by coniferous forests growing downwind from the source. There are three modules: (1) a buoyancy module, (2) a dispersion module, and (3) a foliar absorption module. These modules were used to calculate hourly abovecanopy SO2 concentrations and in-canopy deposition velocities, as well as daily amounts of SO2 absorbed by the forest canopy for downwind distances to 42 km. Model performance testing was done with meteorological data (including ambient SO2 concentrations) collected at various locations downwind from a coal-burning power generator at Grand Lake in central New Brunswick, Canada. Annual SO2 emissions from this facility amounted to about 30,000 tonnes. Calculated SO2 concentrations were similar to those obtained in the field. Calculated SO2 deposition velocities generally agreed with published values.Notation c air parcel cooling parameter (non-dimensional) - E foliar absorption quotient (non-dimensional) - f areal fraction of foliage free from water (non-dimensional) - f w SO2 content of air parcel - h height of the surface layer (m) - H height of the convective mixing layer (m) - H stack stack height (m) - k time level - k drag coefficient of drag on the air parcel (non-dimensional) - K z eddy viscosity coefficient for SO2 (m2·s–1) - L Monin-Obukhov length scale (m) - L A single-sided leaf area index (LAI) - n degree-of-sky cloudiness (non-dimensional) - N number of parcels released with every puff (non-dimensional) - PAR photosynthetically active radiation (W m–2) - Q emission rate (kg s–2) - r b diffusive boundary-layer resistance (s m–1) - r c canopy resistance (s m–1) - r cuticle cuticular resistance (s m–1) - r m mesophyllic resistance (s m–1) - r s stomatal resistance (s m–1) - r exit smokestack exit radius (m) - R normally distributed random variable with mean of zero and variance of t (s) - u * frictional velocity scale, (m s–1) - v lateral wind vector (m s–1) - v d SO2 dry deposition velocity (m s–1) - VCD water vapour deficit (mb) - z can mean tree height (m) - Z zenith position of the sun (deg) - environmental lapse rate (°C m–1) - dry adiabatic lapse rate (0.00986°C m–1) - von Kármán's constant (0.04) - B vertical velocities initiated by buoyancy (m s–1) - canopy extinction coefficient (non-dimensional) - ()a denotes ambient conditions - ()can denotes conditions at the top of the forest canopy - ()h denotes conditions at the top of the surface layer - ()H denotes conditions at the top of the mixed layer - ()s denotes conditions at the canopy surface - ()p denotes conditions of the air parcels  相似文献   

    19.
    Growth in subsonic air traffic over the past 20 years has been dramatic, with an annual increase of }6.1% over the decade between 1978 and 1988. Furthermore, aircraft activities in the year 2000 are predicted to be double those of 1990, with a shift towards more high-flying, longhaul subsonics. Aircraft exhaust gases increase the amount of nitrogen oxides (NO x ) in the upper troposphere/lower stratosphere through injection at cruise altitudes. Given that NO x is instrumental in tropospheric ozone production and stratospheric ozone destruction, it is important to determine the influence of subsonic aircraft NO x emissions on levels of atmospheric ozone. This paper describes calculations designed to investigate the impact that subsonic aircraft may already have had on the atmosphere during the 1980s, run in a 2-D chemical-radiative-transport model. The results indicate a significant increase in upper tropospheric ozone over the decade arising from aircraft emissions. However, when comparing model results with observational data, certain discrepancies appear. Lower stratospheric ozone loss over the 1980s does not appear to be greatly altered by the inclusion of aircraft emissions in the model. However, given the trend in greater numbers of long-haul subsonic aircraft, this factor must be considered in any further calculations.  相似文献   

    20.
    A series of experiments carried out in a pasture field during a growing season, allowed a radiometric determination of the scalar roughness for sensible heatz oh,r . The values ofz oh,r are shown to vary over the range of 10–1–10–7m both diurnally and seasonally, and an existing theoretical model for the estimation of scalar roughness for sensible heat is found to be inappropriate for the precise estimation ofz oh,r . To parameterizez oh,r better, a multiple regression analysis was performed, with predictor candidates such as solar elevation, solar radiationR s , leaf area index LAI, canopy height, the ratio of the solar radiation and the extraterrestrial radiationR s /R e , the ratio of the direct and the total solar radiationR d /R s , and the roughness Reynolds number among others. The best regression equation which usesR s , LAI,R s /R e , andR d /R s is derived withr=0.75; with smaller numbers of predictors, values ofr tend to deteriorate gradually down tor=0.52 when only one predictor, LAI, was incorporated into the equation.  相似文献   

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