鹤山大气超级站旱季单颗粒气溶胶化学特征研究

利用单颗粒气溶胶飞行时间质谱等仪器在鹤山大气超级站开展综合观测,结合ART-2a自适应共振神经网络聚类算法,将2013年11月4日~2013年12月30日期间监测到的1637330个细颗粒分成9类: EC-Fresh颗粒、EC-Nitrate/Sulfate颗粒、K-EC颗粒、Ca-EC颗粒、ECOC颗粒、OC-Levoglucosan颗粒、OC-Nitrate/Sulfate颗粒、K-Nitrate/Sulfate颗粒和Metal-rich颗粒.结果表明:该大气超级站所在地区旱季霾日有利于与水溶性二次无机组分混合的EC-Nitrate/Sulfate颗粒、K-Nitrate/Sulfate颗粒的累积;晴朗天更有利于二次有机组分在气溶胶颗粒中生成,雨天受当地排放源的影响显著,含有较高EC-Fresh和K-EC颗粒.相关性的研究发现,EC-Nitrate/Sulfate颗粒与能见度有良好的相关性,它们对霾的形成有至关重要的作用.     

Chemical composition and size distribution of secondary organic aerosol formed from the photooxidation of isoprene

Photooxidation of isoprene leads to the formation of secondary organic aerosol (SOA). In this study, the chemical composition of SOA formed from OH-initiated photooxidation of isoprene has been investigated with gas chromatography/mass spectrometry (GC/MS) and a home-made aerosol time-of-flight mass spectrometer. Sampling particles generated in a home-made smog chamber. The size distribution of SOA particles was detected by a TSI 3321 aerodynamic particle size spectrometer in real time. Results showed that SOA created by isoprene photooxidation was predominantly in the form of fine particles, which have diameters less than 2.5 m. The obtained mass spectra of individual particles show that products of the OH-initiated oxidation of isoprene contain methyl vinyl ketone, methacrolein, formaldehyde, and some other hydroxycarbonyls. The possible reaction mechanisms leading to these products were also discussed.     

天山乌鲁木齐河源1号冰川气溶胶可溶性离子观测与分析研究

基于2003年、2004年和2007年3年内共采集的155个气溶胶样品的分析测试,探讨了天山乌鲁木齐河源1号冰川区气溶胶中可溶性离子的组成及年际变化特征,并对其可能来源进行了分析.结果表明,气溶胶可溶性离子平均浓度为2.759μg·m-3,化学组成以NO-3、SO2-4、Ca2+和CO2-3为主,冰川区大气环境呈碱性.可溶性离子总质量浓度年际变化特征为2007年2004年2003年,主要离子组成没有发生明显变化,但单一离子浓度变化不尽相同,其原因主要与沙尘活动的强弱有关.Ca2+、Na+、Mg2+、CO2-3和Cl-主要可能来自陆源矿物,而NO-3和NH+4很大程度上以人为源为主;并且发现,SO2-4和K+可能同时受陆地源与人类活动来源的影响.通过气团轨迹聚类分析得出,冰川区大气主要受来自西南方、西方及西北方3个方向气团的控制,这些气团均经过伊犁河谷或阿拉山口到达冰川区,其中,在距地面2000 m以下高度传输的气团会带来大量的沙尘物质,影响冰川区大气环境.     

Role of secondary aerosols in haze formation in summer in the Megacity Beijing

A field experiment from 18 August to 8 September 2006 in Beijing, China, was carried out. A hazy day was defined as visibility < l0 km and RH (relative humidity) < 90%. Four haze episodes, which accounted for ~ 60% of the time during the whole campaign, were characterized by increases of SNA (sulfate, nitrate, and ammonium) and SOA (secondary organic aerosol) concentrations. The average values with standard deviation of SO₄^2 −, NO₃⁻, NH₄⁺ and SOA were 49.8 (± 31.6), 31.4 (± 22.3), 25.8 (± 16.6) and 8.9 (± 4.1) μg/m³, respectively, during the haze episodes, which were 4.3, 3.4, 4.1, and 1.7 times those in the non-haze days. The SO₄^2 −, NO₃⁻, NH₄⁺, and SOA accounted for 15.8%, 8.8%, 7.3%, and 6.0% of the total mass concentration of PM₁₀ during the non-haze days. The respective contributions of SNA species to PM₁₀ rose to about 27.2%, 15.9%, and 13.9% during the haze days, while the contributions of SOA maintained the same level with a slight decrease to about 4.9%. The observed mass concentrations of SNA and SOA increased with the increase of PM₁₀ mass concentration, however, the rate of increase of SNA was much faster than that of the SOA. The SOR (sulfur oxidation ratio) and NOR (nitrogen oxidation ratio) increased from non-haze days to hazy days, and increased with the increase of RH. High concentrations of aerosols and water vapor favored the conversion of SO₂ to SO₄^2 − and NO₂ to NO₃⁻, which accelerated the accumulation of the aerosols and resulted in the formation of haze in Beijing.     

Chemical characterization of size-resolved aerosols in four seasons and hazy days in the megacity Beijing of China

Size-resolved aerosol samples were collected by MOUDI in four seasons in 2007 in Beijing. The PM₁₀ and PM_1.8 mass concentrations were 166.0 ± 120.5 and 91.6 ± 69.7 μg/m³, respectively, throughout the measurement, with seasonal variation: nearly two times higher in autumn than in summer and spring. Serious fine particle pollution occurred in winter with the PM_1.8/PM₁₀ ratio of 0.63, which was higher than other seasons. The size distribution of PM showed obvious seasonal and diurnal variation, with a smaller fine mode peak in spring and in the daytime. OM (organic matter = 1.6 × OC (organic carbon)) and SIA (secondary inorganic aerosol) were major components of fine particles, while OM, SIA and Ca^2 + were major components in coarse particles. Moreover, secondary components, mainly SOA (secondary organic aerosol) and SIA, accounted for 46%–96% of each size bin in fine particles, which meant that secondary pollution existed all year. Sulfates and nitrates, primarily in the form of (NH₄)₂SO₄, NH₄NO₃, CaSO₄, Na₂SO₄ and K₂SO₄, calculated by the model ISORROPIA II, were major components of the solid phase in fine particles. The PM concentration and size distribution were similar in the four seasons on non-haze days, while large differences occurred on haze days, which indicated seasonal variation of PM concentration and size distribution were dominated by haze days. The SIA concentrations and fractions of nearly all size bins were higher on haze days than on non-haze days, which was attributed to heterogeneous aqueous reactions on haze days in the four seasons.     

北京地区对流层低层臭氧及硫酸盐气溶胶的时空分布

基于OMI/Aura卫星资料,分析了北京地区2007~2016年近10a对流层O₃浓度（0~3km）、硫酸盐气溶胶光学厚度（0~2km）、SO₂（边界层以内）柱浓度时空演变特征.结果表明,近10a来北京地区O₃浓度总体呈现上升趋势,最低值在2007年,浓度为33.65 μg/m³;硫酸盐气溶胶污染总体变化呈现先下降后增长的趋势,2007年硫酸盐气溶胶污染最为严重,2011年污染最轻,对应的AOD值为0.252,但在2014年以后,硫酸盐气溶胶污染又出现增长趋势;SO₂浓度在2007~2016年总体呈现下降的变化趋势,且下降趋势明显,最高值为2007年,最低值出现在2016年,最低值比最高值降低了60.42%,但在2011年污染出现反弹.北京O₃季节变化明显,夏季高、春秋次之、冬季低;硫酸盐气溶胶污染季节特征与O₃相同;SO₂污染主要集中在冬季,采暖期污染程度高于非采暖期.     

Pollution sources of atmospheric fine particles and secondary aerosol characteristics in Beijing

To investigate the secondary formation and pollution sources of atmospheric particles in urban Beijing, PM_2.5 and its chemical components were collected and determined by URG-9000D ambient ion monitor (AIM) from March 2016 to January 2017. Among water-soluble ions (WSIs), NO₃^?, SO₄^2- and NH₄⁺ (SNA) had the largest proportion (77.8%) with the total concentration of 23.8 μg/m³. Moreover, as fine particle pollution worsened, the NO₃^?, SO₄^2- and NH₄⁺ concentrations increased basically, which revealed that secondary aerosols were the main cause of particle pollution in Beijing. Furthermore, the particle neutralization ratio (1.1), the ammonia to sulfate molar ratio (3.4) and the nitrate to sulfate molar ratio (2.2) showed that secondary aerosols are under ammonium-rich conditions with the main chemical forms of NH₄NO₃ and (NH₄)₂SO₄, and vehicle emission could be the main anthropogenic source of secondary aerosols in Beijing. Source analysis further indicated that secondary aerosols, solid fuel combustion, dust and marine aerosol were the principal pollution sources of PM_2.5, accounting for about 46.1%, 22.4% and 13.0%, respectively, and Inner Mongolia and Hebei Provinces could be considered as the main potential sources of PM_2.5 in urban Beijing. In addition, secondary formation process was closely related with gaseous precursor emission amounts (SO₂, NO₂, NH₃ and HONO), atmospheric ozone concentration (O₃), meteorological conditions (temperature and relative humidity) and particle components. Sensitive analysis of the thermodynamic equilibrium model (ISORROPIA II) revealed that controlling total nitrate (TN) is the effective measure to mitigate fine particle pollution in Beijing.     

大气气溶胶粒子质量浓度分布规律研究

在可吸入性颗粒物粒径范围内(d_p<10μm),上海市区大气中气溶胶粒子质量浓度分布为双峰型,峰值出现在1.0μm左右(积聚模态粒子区)和4.5μm左右(粗粒子区),且呈现大粒径处峰值大于小粒径处峰值的趋势。与质量浓度分布曲线相似,质量概率密度分布也为双峰型,峰值出现在0.8μm左右和4.0μm左右。模拟结果表明,上海市区大气中气溶胶粒子质量概率密度分布规律符合双重分布函数:y=exp[-(a_4d~4 a_3d~3 a_2d~2 a_1d a_0)],所表征的类型,应用双重分布函数能解释大气气溶胶粒子的分布规律。     

利用风云四、MODIS及CALIPSO卫星资料分析西北沙尘过程的垂直和水平分布特征

FY-4A提供的高时间分辨率沙尘强度产品为分析沙尘过程中气溶胶分布提供了新的思路.本研究使用MODIS暗像元/深蓝/合成算法的AOD产品以及FY-4A沙尘强度产品,分析了2018年春季中国西北地区的两次典型沙尘过程,并使用CALIPSO后向散射系数产品研究了这两次事件中气溶胶的垂直分布特征.研究结果表明：①风云四号沙尘强度产品与MODIS深蓝算法产品以及合成算法产品在西北沙漠地区的沙尘分布情况上具有很好的空间一致性;②对于沙尘有明显向东输送的沙尘过程而言（如2018年4月4—6日）,沙尘主要分布在2~6 km,有些地区甚至只有4 km以上才存在沙尘,在沙尘输送的下游地区,沙尘主要分布在2 km以下的低空;而对于沙尘没有向外扩散的沙尘过程（如2018年5月21—23日）,沙尘粒子则主要分布在0~5 km高度处.     

一种新型流管反应器的设计与表征

介绍了一种用于气溶胶生成机制研究的流管反应器（Jiao-FTR,J-FTR）的设计及表征.借助计算流体力学（CFD）模拟和实验测定,表征了不同进气结构和实验条件下反应器内流场的发展及稳定,移动进气管的喷射效应以及气体和颗粒物在反应器内的平均停留时间.结果表明,预混合段进气方式,主流流量,移动进气管结构及注入流量对J-FTR的流场发展以及气体和颗粒物的停留时间具有较大影响;J-FTR的预混合进气段具有使主流快速过渡为层流的优势,在对称进气条件下,当主流流量不超过8L/min,气流在进入主反应段之前可发展为稳定的层流;当移动进气管使用大内径的直管或径面十字型结构时,可以有效减小或避免移动进气管的喷射效应.以上结果不仅可为使用J-FTR开展大气化学和气溶胶生成机制研究提供重要的实验指导,也可为其他研究者设计FTR,进行流管实验提供借鉴.