影响SO2和NOx气相化学转化率的敏感因子分析

在一个已建立的简化的气相化学模式基础上，本文估算了ＳＯ２和ＮＯＸ的气相化学转化率，进一步研究了影响转化率的敏感因子。结果表明：在典型的大气污染状况和晴天无云的条件下，白天ＳＯ２和ＮＯＸ的平均转化率分别为１．５％／ｈ和１３．８／ｈ，大气温度，太阳高度，水汽混合比以及云厚，云量，云中液态水含量等云物理参数都会对转化率产生不同程度的影响。     

污染源、干沉降和气相化学影响硫沉降的数值研究

利用欧拉型区域硫沉降模式对污染源、干沉降和气相化学等物理化学过程在酸沉降中的作用进行了数值分析。结果表明:排放源的强度和高度影响着污染物的分布和输送,其影响是非线性的。在区域酸沉降模式中,干沉降速度和气相化学转化率简单地取为常数对SO#-[2]及SO#+[2-]#-[4]浓度分布引起的误差是不可忽视的。     

中国的酸雨模拟及控制对策研究

本文以大气污染源、大气污染特征、降水化学特征和酸雨污染特征等方面论述了我国在气污染和酸雨污染属于“煤烟型”,并将我国的大气了环境状况与世界其它一些国家作了比较分析。进一步利用我们发展的南京大学酸沉降模式系统（ＮＪＵＡＤＭＳ）模拟了中国地区的ＳＯ２地面浓度和硫沉降分布,并与实际观测浆和亚洲酸雨模式（ＲＡＩＮＳ－ＡＳＬＡ）的计算结果作了比较。最后从能源结构和经济发展状况出发,论述了我国控制ＳＯ２污染和     

区域酸性沉降的数值研究 I. 模式

建立了一个三维时变的欧拉型区域酸性污染物沉降模式，模式包括源排放、平流输送、湍流扩散、干沉积、气相化学、液相化学及湿清除等六大部分。考虑到计算条件的承受能力和应用性的要求，在把握酸沉降形成的关键过程的前提下，合理地简化设计模式。相对于国内已有的工作，本模式在干沉积、气相化学、液相化学和湿清除等方面均有所改进。     

欧拉型区域硫沉降模式研究

建立了一个三维硫沉降欧拉模式，模式中比较全面地考虑了硫沉降过程中的物理、化学机制。包括平流、扩散、干湿沉降和积云的垂直输送作用等物理过程，气相化学、液相化学和气溶胶表面的非均相化学等化学过程。其中非均相化学和积云的垂直输送参数化在国内外同类模式中尚不多见。模式结果与实测及其他模式结果的对比表明，该模式能够较好地模拟出SO2的水平和垂直分布及SO2-4在降水中的浓度。     

中国西南和华南地区硫沉降数值模拟

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。     

硫化物的云下清除

采用硫化物清除的化学模式模拟计算ＳＯ２的云下清除过程,既考虑了ＳＯ２在雨滴中的溶解和电离作用,也考虑了Ｓ（Ⅳ）与氧化剂Ｈ２Ｏ２之间的化学反应。由模式分别给出了空气中ＳＯ２浓度的时空变化和雨滴中Ｓ（Ⅳ）浓度的时空变化。     

用STEM—Ⅱ模式研究东亚地区春季沙尘气溶胶对硫化物输送和沉降的影响

利用ＳＴＥＭ－ＩＩ三维区域尺度大气化学模式,研究了１９９４年３月１日至１４日东亚地区春季沙尘气溶胶对硫化物输送和沉降的影响。结果表明,ＳＯ２和ＳＯ２４的大值区主要出现在我国东部地区。在模拟时段,日本地区火山源的排放对该地区大气中Ｓ分布的贡献达１０％～３０％。并与当时飞机的观测结果相吻合。模拟区域内ＳＯ２和ＳＯ２４的收支的分析研究表明,在硫的总排放量中,从东边界面流出去的输送通量最大,并出现在３０～４００Ｎ带的２～６ｋｍ高度上,这是与该地区最大的人为排放源所在地相一致的。最后,给出了模拟时段整个对流层大气ＳＯ２－４气溶胶含量的分布,还仨算了ＳＯ２－４气溶胶对地气系统的直接辐射强迫和温度变化的影响。     

区域酸沉降模式

本文提出一个区域的欧拉酸雨模式,包括了大气中污染物质的输送、扩散、非线性化学转化和干湿沉降等物理和化学过程.气相化学反应有18种化学物质,包含了二氧化硫气相氧化的主要化学方程.液相氧化反应包含了H_2O_2,O_3及催化剂对二氧化硫的氧化过程.水平方向有35×35个网格点,垂直方向分15层.选用了四川、贵州地区1988年的8次降水过程对模式作了检验,结果证明模式能较好地模拟这个地区的二氧化硫、硫酸根及降水pH的分布状况.     

西太平洋区域二甲硫酸及其他硫化物的模拟研究

本文利用一维光化学模式，以二甲硫醚（ＤｉｍｅｔｈｙｌＳｕｌｆｉｄｅ，简称ＤＭＳ）为源模拟了西太平洋对流层的硫化物循环。ＤＭＳ海－气通量由“ｓｔａｇｎａｎｔ－ｆｉｌｍ”模式进行计算。尽管海洋大气中ＯＣＳ浓度比ＤＭＳ大一个量级，但它对ＳＯ２的贡献很小，ＤＭＳ仍是海洋大气中ＳＯ２的主要源。在大气垂直湍流输送过程中，ＤＭＳ白天与ＯＨ反应，夜间与ＮＯ３反应被氧化成ＳＯ２，ＳＯ２大部分通过非均相转化形成Ｈ２ＳＯ４。模拟结果与ＰＥＭ－ＷＥＳＴ－Ａ观测资料对比，取得了较好的一致性。     

Numerical Simulation on the Rainout-Removal of Sulfur Dioxide and Acidification of Precipitation from Stratiform Clouds

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 fac-tors, 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 rate S(IV)－S (VI) and the wet deposition rate of SO2 are discussed.     

积云的清除作用与其酸化的数值模拟

一维时变参数化积云模式与污染物浓度连续方程相结合，根据积云内外SO2和HNO3浓度、云水S(VI)浓度、H2O2和O3的氧化速率以及地面雨水S(VI)浓度的时空变化，分别讨论核化清除、液相氧化、云下气溶胶清除、碱性气溶胶、云外污染物的夹卷以及SO2初始分布等因子的重要性。     

PRIMARY STUDY OF SULFATE AND CARBONACEOUS AEROSOLS IN BEIJING

Results of our aerosol study, performed during 1983-1984 in Beijing, demonstrate that ambient carbonaceous aerosols are derived mainly from coal combustion. Different SO, oxidation processes have been observed in summer and winter. The winter sulfate appears to be produced locally and associated with products of incomplete combustion.     

Anthropogenic Effects on Biogenic Secondary Organic Aerosol Formation

Anthropogenic emissions alter biogenic secondary organic aerosol(SOA) formation from naturally emitted volatile organic compounds(BVOCs). We review the major laboratory and field findings with regard to effects of anthropogenic pollutants(NOx, anthropogenic aerosols, SO_2, NH_3) on biogenic SOA formation. NOx participate in BVOC oxidation through changing the radical chemistry and oxidation capacity, leading to a complex SOA composition and yield sensitivity towards NOx level for different or even specific hydrocarbon precursors. Anthropogenic aerosols act as an important intermedium for gas–particle partitioning and particle-phase reactions, processes of which are influenced by the particle phase state, acidity, water content and thus associated with biogenic SOA mass accumulation. SO_2 modifies biogenic SOA formation mainly through sulfuric acid formation and accompanies new particle formation and acid-catalyzed heterogeneous reactions. Some new SO_2-involved mechanisms for organosulfate formation have also been proposed.NH_3/amines, as the most prevalent base species in the atmosphere, influence biogenic SOA composition and modify the optical properties of SOA. The response of SOA formation behavior to these anthropogenic pollutants varies among different BVOCs precursors. Investigations on anthropogenic–biogenic interactions in some areas of China that are simultaneously influenced by anthropogenic and biogenic emissions are summarized. Based on this review, some recommendations are made for a more accurate assessment of controllable biogenic SOA formation and its contribution to the total SOA budget. This study also highlights the importance of controlling anthropogenic pollutant emissions with effective pollutant mitigation policies to reduce regional and global biogenic SOA formation.     

The Role of Multiphase Chemistry in the Oxidation of Dimethylsulphide (DMS). A Latitude Dependent Analysis

A kinetic model for the OH-initiated homogeneous gas phase oxidation of dimethylsulfide (DMS) in the atmosphere (Saltelli and Hjorth, 1995), has been extended here to include the liquid phase chemistry. The updated model has then been employed to predict the temperature dependency of the MSA/nss-SO42- ratio. Model predictions have been compared with observational data reported in Bates et al. (1992). Sensitivity and uncertainty analysis has been performed in a Monte Carlo fashion to identify which are the important uncertainties on the input parameters and which are the possible combinations of parameter values that could explain the field observations. Results of the analysis have indicated that the temperature dependencies of the interactions between gas phase and liquid phase chemistry may to a large extent explain the observed T-dependence of the MSA/nss- SO42- ratio. The potential role of multi-phase atmospheric chemistry, not only in the case of SO2 but also of other oxidation products of DMS and, particularly, of DMS itself, has been highlighted.     

Characteristics of Anthropogenic Sulfate and Carbonaceous Aerosols over East Asia： Regional Modeling and Observation

The authors present spatial and temporal characteristics of anthropogenic sulfate and carbonaceous aerosols over East Asia using a 3-D coupled regional climate-chemistry-aerosol model, and compare the simulation with the limited aerosol observations over the region. The aerosol module consists of SO2, SO4^2-, hydrophobic and hydrophilic black carbon （BC） and organic carbon compounds （OC）, including emission, advections, dry and wet deposition, and chemical production and conversion. The simulated patterns of SO2 are closely tied to its emission rate, with sharp gradients between the highly polluted regions and more rural areas. Chemical conversion （especially in the aqueous phase） and dry deposition remove 60% and 30% of the total SO2 emission, respectively. The SO4^2- shows less horizontal gradient and seasonality than SO2, with wet deposition （60%） and export （27%） being two major sinks. Carbonaceous aerosols are spatially smoother than sulfur species. The aging process transforms more than 80% of hydrophobic BC and OC to hydrophilic components, which are removed by wet deposition （60%） and export （30%）. The simulated spatial and seasonal SO4^2-, BC and OC aerosol concentrations and total aerosol optical depth are generally consistent with the observations in rural areas over East Asia, with lower bias in simulated OC aerosols, likely due to the underestimation of anthropogenic OC emissions and missing treatment of secondary organic carbon. The results suggest that our model is a useful tool for characterizing the anthropogenic aerosol cycle and for assessing its potential climatic and environmental effects in future studies.     

新标准下空气质量预报指导产品对比检验

为了解和掌握上级指导产品对石家庄市空气质量预报的适用性,进一步提高石家庄市空气质量预报的准确性,利用国家气象中心(NMC)、北京区域气象中心(BJ)和河北省气象局(HB)空气质量预报产品,对石家庄市夏季4种主要污染物PM_(2.5)、PM_(10)、O_3和SO_2的预报进行了对比检验,结果表明:1)NMC对4种污染物的预报效果均逊于HB和BJ的,对PM_(10)、PM_(2.5)和SO_2的预报值明显较实况偏大,尤其在发生重污染天气时,对PM_(10)和PM_(2.5)的空报率高达90%以上;2)HB对PM_(10)和SO_2的预报效果好于BJ的,对SO_2的预报值与实况值均在一个等级范围内,发生重污染天气时,对PM_(10)的预报效果好于BJ的,预报值更接近于实况,但对重污染向优、良转折天气的预报值偏高;3)BJ预报PM_(2.5)和O_3的效果好于HB的,对O_3的0级误差级别预报准确率高达90.5%,对PM_(2.5)优到轻度污染等级的预报效果较好,但对重污染天气的预报值低于实况。     

我国西部清洁大气中SO2 和NO2的观测和分析

在我国青海省瓦里关大气本底基准观象台（海拔3810 m,100°54′E,36°17′N）,利用浸渍膜法采集大气中的SO2和NO2，使用离子色谱分析其浓度。1994年8月至1995年7月的测量结果表明，SO2和NO2的平均浓度分别为0.147×10-9和0.055×10-9,SO2和NO2两者具有较好的相关性，其相关系数r=0.87,它们的平均比值为2.6左右。SO2和NO2的浓度受季节和风向的影响，偏东风时浓度较高，偏西风时浓度较低。冬季SO2和NO2的浓度水平较低，而夏季浓度较高。     

北京冬季二氧化硫污染和气象条件的关系

利用2000年1月25日～2月3日北京地区冬季二氧化硫体积分数的梯度监测资料,结合北京325m气象塔的同期气象资料,分析了观测期间北京地区二氧化硫的体积分数变化趋势及垂直分布情况,讨论了大气二氧化硫体积分数变化和气象条件的关系及二氧化硫的来源问题.研究表明:二氧化硫的体积分数变化及垂直输送与风速、风向、大气稳定度密切相关.风速越小,大气越稳定,近地层大气的二氧化硫污染就越严重;当北京冬季吹SSW、SW、WSW和W风时有较高的二氧化硫.