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积云对二氧化硫和硫酸盐气溶胶作用的研究 总被引：1，自引：1，他引：0
利用一个冰雹云模式与云化学模式耦合而成的二维积云化学模式,研究对流云的输送、微物理转化、云内化学过程、湿清除对SO2及硫酸盐气溶胶的作用。云化学模式的结果表明,由于SO2在向上输送的过程中可溶解于云水和雨水中,从而阻止了SO2向上部的转移,因此对气相SO2来说,云的输送是一个相当无效的过程,而液相清除起主要作用。硫酸盐气溶胶的收支分析表明,降水清除了1.67 mol的SO2-4,占气溶胶总量的64%,其中液态降水清除了0.72 mol,固态降水清除了0.95 mol,说明了冰相过程在硫沉降中的重要性。 相似文献
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全球人为硫酸盐和烟尘气溶胶资料及其光学厚度的分布特征 总被引：8，自引：3，他引：5
简单介绍了两种不同化学输送模式及其输出的硫酸盐和/或烟尘气溶胶资料,初步分析了它们之间的异同。同时,在广泛搜集整理已有资料的基础上,给出了硫酸盐和烟尘气溶胶在整个太阳光谱0.2～40 μm波段内共72个间隔上的复折射指数资料;计算并分析了其整层光学厚度的全球分布特征。结果表明,无论是地理分布还是数值大小均基本合理。结合上述资料及计算结果,初步建立了一个全球硫酸盐和烟尘气溶胶资料库,该库对化学输送模式、辐射强迫和气候效应的研究都有参考意义。 相似文献
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东亚地区春季二氧化硫的输送与转化过程研究I.模式及其验证 总被引：5，自引：0，他引：5
结合新近评估的东亚地区污染源资料,作者利用一个耦合的区域化学输送模式系统以探讨东亚地区春季期间气象过程、气相与液相化学过程、非均相化学过程、气溶胶过程和干湿沉降过程对二氧化硫输送及转化过程的影响,并研究二氧化硫和硫酸盐气溶胶的空间分布及变化特征.模拟的二氧化硫和硫酸盐气溶胶的浓度值与2001年春季飞机和地面获取的观测值进行了比较.比较结果显示,模拟值与观测值具有很好的一致性,模式系统很好地反映了二氧化硫和硫酸盐气溶胶的分布特征和变化规律,再现了许多观测到的重要特征,为进一步分析模拟结果奠定了基础. 相似文献
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结合新近评估的东亚地区污染源资料，作者利用一个耦合的区域化学输送模式系统以探讨东亚地区春季期间气象过程、气相与液相化学过程、非均相化学过程、气溶胶过程和干湿沉降过程对二氧化硫输送及转化过程的影响，并研究二氧化硫和硫酸盐气溶胶的空间分布及变化特征。模拟的二氧化硫和硫酸盐气溶胶的浓度值与2001年春季飞机和地面获取的观测值进行了比较。比较结果显示，模拟值与观测值具有很好的一致性，模式系统很好地反映了二氧化硫和硫酸盐气溶胶的分布特征和变化规律，再现了许多观测到的重要特征，为进一步分析模拟结果奠定了基础。 相似文献
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利用CMAQ(Community Multi-scale Air Quality)模式模拟了中国西南和华南地区的硫沉降。模式中详细考虑了气象过程、气相与液相化学过程、非均相化学过程、气溶胶过程和干湿沉降过程对SO2输送、转化和沉降过程的影响。通过与IMPACTS小流域的观测资料的比较,显示了该模式系统能够较好地模拟SO2在大气中的转化以及干湿沉降过程。在此基础之上,分析了不同季节该区域的硫沉降和向外输送的情况,并且模拟了该区域2002年全年的硫沉降分布状况,这为该区域有效地污染治理奠定了基础。 相似文献
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相对湿度对气溶胶辐射特性和辐射强迫的影响 总被引：14，自引：4，他引：14
采用已有的气溶胶折射指数等资料 ,计算了在不同的相对湿度条件下硫酸盐气溶胶的辐射特性。结合两种不同化学输送模式 (CTM )的模拟结果及LASGGOALS/AGCM模式 ,模拟估算了考虑相对湿度影响后全球硫酸盐气溶胶的辐射强迫。结果表明 :(1)随着相对湿度的增加 ,硫酸盐气溶胶的质量消光效率因子在短波波段有所减小 ,单次散射反照率仅在长波波段有所增加 ,不对称因子在整个波段均有所增加 ;(2 )用两个CTM资料模拟辐射强迫的结果相差较大 ,其全球平均辐射强迫分别为 - 0 .2 6 8和 - 0 .816W/m2 ;(3)在考虑相对湿度的影响后 ,硫酸盐气溶胶辐射强迫的分布类型与相应干粒子的强迫分布类型基本相同 ,但全球平均的强迫值减少了 6 %左右。 相似文献
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东亚地区春季硫氧化物浓度分布及其收支研究 总被引：2，自引：0，他引：2
利用一个耦合的区域化学输送模式系统,模拟了2001年3~4月间东亚区域二氧化硫(SO2)和硫酸盐(SO42-)气溶胶浓度的时空分布,并分析了它们的来源、输送、转化和沉降过程在浓度形成中的作用。为了检验模拟结果的合理性,侧重分析了4月9~12日SO2的输送和转化过程。在这一期间,SO2浓度观测资料显示,日本的观测站Happo、Oki和Hedo周围及日本海部分海域先后经历了一次SO2浓度高值。模拟结果表明,日本东京附近的三宅岛火山喷发严重影响了日本列岛和周边海域SO2和SO42-气溶胶的分布,是引起观测站周围及日本海部分海域SO2浓度高值的主要原因。3月1日至4月31日间的硫收支分析显示,气相与液相化学过程在SO2的氧化过程中具有同等的重要性,模拟区域排放的硫氧化物中有约42%(其中约25%为SO2)被输送到模拟区域以外,约57%(约35%为湿沉降)沉积在模拟区域内。 相似文献
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东亚地区沙尘气溶胶影响硫酸盐形成的模式评估 总被引：14，自引：0，他引：14
利用STEM-II三维区域大气化学模式,耦合沙尘气溶胶表面相过程,研究了1994年3月1日至14日间东亚地区沙尘气溶胶对硫酸盐形成的影响。结果表明,SO2气体在沙尘气溶胶表面上进行的非均相氧化过程是硫酸盐形成的一条重要途径,由这条途径提供的硫酸盐占其总浓度的20%～50%。 并发现在模拟时段,沙尘暴过程主要影响沙尘源地下游的中国东部地区硫酸盐的分布,使得那里的硫酸盐浓度增加60%以上。 相似文献
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中国地区硫酸盐气溶胶的第一间接气候效应研究 总被引：14，自引：6，他引：8
将区域气候模式(RegCM3)与对流层大气化学模拟(TACM)耦合,建立区域气候化学模拟系统(RegCCMS),用以模拟中国地区硫酸盐气溶胶的空间分布、第一间接辐射强迫及其气候效应。研究结果表明,中国地区硫酸盐气溶胶主要集中在四川、河南、山东等地,秋冬季浓度较高而夏季浓度较低。1月份浓度最高值中心在四川,最高达到50μg/m3,而7月则出现在河南等地,浓度最高达10μg/m3。1、4、7、10月硫酸盐气溶胶的第一间接辐射强迫全国平均值分别为-1.80、-2.75、-3.43、-1.83 W/m2,局部地区可达-12 W/m2。敏感性试验结果表明,硫酸盐气溶胶的第一间接效应引起气温降低,降水减少,在不同季节和地区气温和降水的变化存在明显差异。 相似文献
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By C. R. HOYLE G. MYHRE I. S. A. ISAKSEN 《Tellus. Series B, Chemical and physical meteorology》2009,61(4):618-624
The effect of anthropogenic emissions from China on global burdens of ozone, sulphate, organic carbon (OC) and black carbon (BC) aerosols is examined, using the three-dimensional chemistry transport model Oslo CTM2. Two model simulations were performed, the first with global present-day emissions and the second with the anthropogenic emissions from China set to their pre-industrial levels. The global radiative forcing for these species is then calculated. Industrial emissions from China are found to account for a 4–5% increase in the global burden of OC aerosol, the change in secondary organic aerosol being slightly less than that of primary organic aerosol. A 10% increase in the global sulphate aerosol burden is calculated, and the increase in BC is 23%. The global radiative forcing of aerosols from China was calculated to be −62, −3.7, −13 and 89 mW m−2 , for sulphate, secondary organic, primary organic and BC aerosols, respectively. The increase in ozone causes a forcing of 77 mW m−2 . 相似文献
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Abstract Aqueous‐phase H2O2 production in a rainband and its possible effect on sulphate production are studied by means of a two‐dimensional numerical model. In‐cloud peroxide production is incorporated into this chemistry model and its simulation results are compared with those in which aqueous‐phase H2O2 came only from the dissolution of gaseous H2O2 from the cloud interstitial air. Results are presented for two different polluted situations ‐ Case 1 having initial SO2 and sulphate aerosol profiles representative of a moderately polluted air mass, and Case 2 having chemical profiles expected to increase the relative importance of oxidation to nucleation as a means of contributing sulphate to cloud and rain. Sulphate production increased in both cases, although in Case 1 the effect of this increase on the concentration of sulphate in rain is negligible because nucleation and scavenging of aerosol are the major processes by which sulphate enters cloud and rain. In Case 2, sulphate concentrations in rain increase by 5–10%. Under environmental conditions of low sulphate aerosol, where oxidation reactions are the dominant means for sulphate to enter cloud and rain, the neglect of sulphate produced by the additional H2O2 may lead to error. The usual uncertainties in the initial SO2 and sulphate aerosol vertical profiles, however, could be a more significant source of error in simulations of the chemistry of cloud and precipitation than the neglect of aqueous‐phase peroxide production during the lifetime of even a long‐lived system. 相似文献
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Climatic changes associated with a global “2°C-stabilization” scenario simulated by the ECHAM5/MPI-OM coupled climate model 总被引：1，自引：0，他引：1
Wilhelm May 《Climate Dynamics》2008,31(2-3):283-313
In this study, concentrations of the well-mixed greenhouse gases as well as the anthropogenic sulphate aerosol load and stratospheric ozone concentrations are prescribed to the ECHAM5/MPI-OM coupled climate model so that the simulated global warming does not exceed 2°C relative to pre-industrial times. The climatic changes associated with this so-called “2°C-stabilization” scenario are assessed in further detail, considering a variety of meteorological and oceanic variables. The climatic changes associated with such a relatively weak climate forcing supplement the recently published fourth assessment report by the IPCC in that such a stabilization scenario can only be achieved by mitigation initiatives. Also, the impact of the anthropogenic sulphate aerosol load and stratospheric ozone concentrations on the simulated climatic changes is investigated. For this particular climate model, the 2°C-stabilization scenario is characterized by the following atmospheric concentrations of the well-mixed greenhouse gases: 418 ppm (CO2), 2,026 ppb (CH4), and 331 ppb (N2O), 786 ppt (CFC-11) and 486 ppt (CFC-12), respectively. These greenhouse gas concentrations correspond to those for 2020 according to the SRES A1B scenario. At the same time, the anthropogenic sulphate aerosol load and stratospheric ozone concentrations are changed to the level in 2100 (again, according to the SRES A1B scenario), with a global anthropogenic sulphur dioxide emission of 28 TgS/year leading to a global anthropogenic sulphate aerosol load of 0.23 TgS. The future changes in climate associated with the 2°C-stabilization scenario show many of the typical features of other climate change scenarios, including those associated with stronger climatic forcings. That are a pronounced warming, particularly at high latitudes accompanied by a marked reduction of the sea-ice cover, a substantial increase in precipitation in the tropics as well as at mid- and high latitudes in both hemispheres but a marked reduction in the subtropics, a significant strengthening of the meridional temperature gradient between the tropical upper troposphere and the lower stratosphere in the extratropics accompanied by a pronounced intensification of the westerly winds in the lower stratosphere, and a strengthening of the westerly winds in the Southern Hemisphere extratropics throughout the troposphere. The magnitudes of these changes, however, are somewhat weaker than for the scenarios associated with stronger global warming due to stronger climatic forcings, such as the SRES A1B scenario. Some of the climatic changes associated with the 2°C-stabilization are relatively strong with respect to the magnitude of the simulated global warming, i.e., the pronounced warming and sea-ice reduction in the Arctic region, the strengthening of the meridional temperature gradient at the northern high latitudes and the general increase in precipitation. Other climatic changes, i.e., the El Niño like warming pattern in the tropical Pacific Ocean and the corresponding changes in the distribution of precipitation in the tropics and in the Southern Oscillation, are not as markedly pronounced as for the scenarios with a stronger global warming. A higher anthropogenic sulphate aerosol load (for 2030 as compared to the level in 2100 according to the SRES A1B scenario) generally weakens the future changes in climate, particularly for precipitation. The most pronounced effects occur in the Northern Hemisphere and in the tropics, where also the main sources of anthropogenic sulphate aerosols are located. 相似文献
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MIHALIS LAZARIDIS SASTRY S. ISUKAPALLI PANOS G. GEORGOPOULOS 《Tellus. Series B, Chemical and physical meteorology》2001,53(1):83-93
A modelling platform for studying photochemical gaseous and aerosol phase processes from localized (e.g., point) sources has been presented. The current approach employs a reactive plume model which extends the regulatory model RPM‐IV by incorporating aerosol processes and heterogeneous chemistry. The physics and chemistry of elemental carbon, organic carbon, sulfate, nitrate, ammonium material of aerosols are treated and attributed to the PM size distribution. A modified version of the carbon bond IV chemical mechanism is included to model the formation of organic aerosol. Aerosol dynamics modeled include mechanisms of nucleation, condensation, dry deposition and gas/particle partitioning of organic matter. The model is first applied to a number of case studies involving emissions from point sources and sulfate particle formation in plumes. Model calculations show that homogeneous nucleation is an efficient process for new particle formation in plumes, in agreement with previous field studies and theoretical predictions. In addition, the model is compared with field data from power plant plumes with satisfactory predictions against gaseous species and total sulphate mass measurements. Finally, the plume model is applied to study secondary organic matter formation due to various emission categories such as vehicles and the oil production sector. 相似文献
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Anthony J. Dore Douglas W. Johnson Simon R. Osborne Thomas W. Choularton Keith N. Bower Meinrat O. Andreae Brian J. Bandy 《Tellus. Series B, Chemical and physical meteorology》2000,52(2):452-462
The second Aerosol Characterisation Experiment (ACE‐2) was aimed at investigating the physical, chemical and radiative properties of aerosol and their evolution in the North Atlantic region. In the 2nd "Lagrangian" experiment, an air mass was tracked over a 30‐h period during conditions of extensive stratocumulus cover. Boundary‐layer measurements of the aerosol size distribution obtained with a passive cavity aerosol spectrometer probe (PCASP) during the experiment show a gradual growth in size of particles in the 0.1–0.2 μm diameter mode. Simultaneously, SO2 concentrations were found to decrease sharply from 800 to 20 ppt. The fraction of sulphate in aerosol ionic mass increased from 0.68±0.07 to 0.82±0.09 for small particles (diameter below 1.7 μm) and from 0.21±0.04 to 0.34±0.03 for large particles (diameter above 1.7 μm). The measurements were compared with a multicyclic parcel model of gas phase diffusion into cloud droplets and aqueous phase chemical reactions. The model was able to broadly reproduce the observed transformation in the aerosol spectra and the timescale for the transformation of SO2 to sulphate aerosol. The modelled SO2 concentration in the boundary layer fell to below half its initial value over a 6.5‐h time period due to a combination of the entrainment of cleaner tropospheric air and cloud chemical reactions. NH3 and HCl gas were also found to play an important rôle in cloud processing in the model. 相似文献
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不同云滴数浓度参数化方案对硝酸盐气溶胶
第一间接效应影响的比较研究 总被引：1，自引：1，他引：0
在区域气候化学模式系统（RegCCMS）中,分别采用Hegg、Hansen、Ghan、Jones等4种云滴数浓度参数化方案,模拟研究了2003年10月硝酸盐气溶胶的浓度分布和第一间接气候效应,并对不同方案进行比较。结果表明,不同方案模拟的硝酸盐气溶胶分布大体上一致,主要集中在河南、山东、河北、四川等地,地面浓度最大值达18 μg/m3。Hegg、Hansen、Ghan、Jones等 4种云滴数浓度参数化方案计算得到的由硝酸盐气溶胶所造成的第一间接辐射强迫全国平均值分别为-148、-205、-161和-140 W/m2。4种方案模拟的硝酸盐气溶胶间接效应都表现为近地面气温下降,降水减少,其中Hansen方案的间接效应最强,Ghan、Hegg方案次之,Jones方案最弱。 相似文献
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The authors used a high-resolution regional climate model(RegCM3) coupled with a chemistry/aerosol module to simulate East Asian climate in 2006 and to test the climatic impacts of aerosols on regionalscale climate.The direct radiative forcing and climatic effects of aerosols(dust,sulfate,black carbon,and organic carbon) were discussed.The results indicated that aerosols generally produced negative radiative forcing at the top-of-the-atmosphere(TOA) over most areas of East Asia.The radiative forcing induced by aerosols exhibited significant seasonal and regional variations,with the strongest forcing occurring in summer.The aerosol feedbacks on surface air temperature and precipitation were clear.Surface cooling dominated features over the East Asian continental areas,which varied in the approximate range of-0.5 to-2°C with the maximum up to-3-C in summer over the deserts of West China.The aerosols induced complicated variations of precipitation.Except in summer,the rainfall generally varied in the range of-1 to 1 mm d-1 over most areas of China. 相似文献
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R. G. Derwent W. J. Collins M. E. Jenkin C. E. Johnson D. S. Stevenson 《Journal of Atmospheric Chemistry》2003,44(1):57-95
A global 3-D Lagrangian chemistry-transport model STOCHEM is used to describe the tropospheric distributions of four components of the secondary atmospheric aerosol: nitrate, sulphate, ammonium and organic compounds. The model describes the detailed chemistry of the formation of the acid precursors from the oxidation of SO2, DMS, NOx, NH3 and terpenes and their uptake into the aerosol. Model results are compared in some detail with the available surface observations. Comparisons are made between the global budgets and burdens found in other modelling studies. The global distributions of the total mass of secondary aerosols have been estimated for the pre-industrial, present day and 2030 emissions and large changes have been estimated in the mass fractions of the different secondary aerosol components. 相似文献
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将区域气候模式（RegCM3）与对流层大气化学模式（TACM）耦合, 建立区域气候化学模拟系统（RegCCMS）, 用以模拟研究中国地区黑碳气溶胶的空间分布、 第一间接辐射强迫及其气候效应。利用RegCCMS模式对2003年1月和7月进行模拟, 结果表明, 我国黑碳气溶胶主要集中在四川、 河北、 山东等地, 1月份浓度最高值中心在四川, 达到4 μg·m-3; 而在7月则出现在华中地区, 高值中心值为3.5 μg·m-3。地面浓度的季节差异不是很明显。1月和7月由黑碳气溶胶所造成的第一间接辐射强迫全国平均值分别为-0.389 W·m-2和-1.18 W·m-2, 局部地区达到-4～-4.5 W·m-2。敏感性试验结果表明, 考虑黑碳气溶胶的第一间接气候效应后, 使得近地面气温下降, 降水减少, 1月变化的平均值分别为-0.025K和-0.0027 mm·d-1, 7月变化的平均值分别为-0.16K和-0.095 mm·d-1, 在不同季节和地区, 气温和降水的变化存在明显差异。 相似文献