Atmospheric photochemistry and secondary aerosol formation of urban air in Lyon, France

Photochemical aging of volatile organic compounds (VOCs) in the atmosphere is an important source of secondary organic aerosol (SOA). To evaluate the formation potential of SOA at an urban site in Lyon (France), an outdoor experiment using a Potential Aerosol Mass (PAM) oxidation flow reactor (OFR) was conducted throughout entire days during January-February 2017. Diurnal variation of SOA formations and their correlation with OH radical exposure (OHexp), ambient pollutants (VOCs and particulate matters, PM), Relative Humidity (RH), and temperature were explored in this study. Ambient urban air was exposed to high concentration of OH radicals with OHexp in range of (0.2–1.2)×10¹² molecule/(cm³?sec), corresponding to several days to weeks of equivalent atmospheric photochemical aging. The results informed that urban air at Lyon has high potency to contribute to SOA, and these SOA productions were favored from OH radical photochemical oxidation rather than via ozonolysis. Maximum SOA formation (36 µg/m³) was obtained at OHexp of about 7.4 × 10¹¹molecule/(cm³?sec), equivalent to approximately 5 days of atmospheric oxidation. The correlation between SOA formation and ambient environment conditions (RH & temperature, VOCs and PM) was observed. It was the first time to estimate SOA formation potential from ambient air over a long period in urban environment of Lyon.     

黄渤海上空气溶胶类型判别及其成因分析

气溶胶是大气环境的重要组成部分,其对天气和气候变化有重要影响,对人类健康也有危害.对气溶胶类型的区分有利于判别气溶胶的来源,这对控制气溶胶污染源、改善区域环境质量有重要的推动作用.本文基于黄渤海区域6个观测点的实测数据和卫星遥感数据,采用聚类分析方法对黄渤海上空的气溶胶进行分类,并采用拉格朗日轨迹追踪法判定气溶胶的来源.研究发现,黄渤海上空的气溶胶类型以清洁大陆型和生物燃烧以及城市/工业型为主,陆源输入是黄渤海上空气溶胶的重要来源.清洁大陆型的气溶胶在黄海中部的贡献率相比于其余海域偏低,这也间接表明近岸的气溶胶更易受到来自陆地的影响,离岸区域受陆地的影响相对较小.     

Investigation on condensable particulate matter emission characteristics in wet ammonia-based desulfurization system

Particulate matter emissions from ammonia-based wet flue gas desulfurization (Ammonia-WFGD) systems are composed of a filterable particulate matter and a condensable particulate matter (CPM) portion. However, the CPM part has been ignored for a long time, which results in an underestimation of the aerosol problems caused by Ammonia-WFGD systems. In our research, the characteristics of the CPM that emits from an Ammonia-WFGD system are investigated experimentally for the first time, with the US Environmental Protection Agency Method 202 employed as the primary measurement. The influences of some essential desulfurizing parameters are evaluated based on the experimental data. The results show that CPM contributes about 68.8% to the total particulate matter emission. CPM consists mainly of ammonium sulfates/sulfites, with the organic part accounting for less than 4%. CPM is mostly in the submicron fraction, about 71.1% of which originates from the NH₃–H₂O–SO₂ reactions. The appropriate adjustments for the parameters of the flue gas and the desulfurizing solution can inhibit CPM formation to different extents. This indicates that the parameter optimizations are promising in solving CPM emission problems in Ammonia-WFGD systems, in which the pH adjustment alone can abate CPM emission by around 49%. The opposite variations of the parameters need attention because they can cause tremendous CPM emission increase.     

Pollutants identification of ambient aerosols by two types of aerosol mass spectrometers over southeast coastal area, China

Two different aerosol mass spectrometers, Aerodyne Aerosol Mass Spectrometer(AMS) and Single Particle Aerosol Mass Spectrometer(SPAMS) were deployed to identify the aerosol pollutants over Xiamen, representing the coastal urban area. Five obvious processes were classified during the whole observation period. Organics and sulfate were the dominant components in ambient aerosols over Xiamen. Most of the particles were in the size range of 0.2–1.0 μm, accounting for over 97% of the total particles measured by both instruments.Organics, as well as sulfate, measured by AMS were in good correlation with measured by SPAMS. However, high concentration of NH4+was obtained by AMS, while extremely low value of NH4+was detected by SPAMS. Contrarily, high particle number counts of NO3-and Clwere given by SPAMS while low concentrations of NO3-and Cl-were measured by AMS. The variations of POA and SOA obtained from SPAMS during event 1 and event 2 were in accordance with the analysis of HOA and OOA given by AMS, suggesting that both of AMS and SPAMS can well identify the organic clusters of aerosol particles. Overestimate or underestimate of the aerosol sources and acidity would be present in some circumstances when the measurement results were used to analyze the aerosol properties, because of the detection loss of some species for both instruments.     

基于FY-4A卫星数据反演气溶胶光学厚度及分析应用

风云四号A星（FY-4A）是我国新一代静止气象卫星,多通道扫描成像辐射计（AGRI）是风云四号静止气象卫星的主要载荷之一.为探究FY4A数据用于气溶胶光学厚度（AOD）反演的可行性,基于FY-4A/AGRI数据,利用暗像元算法对2019年2月23~26日及10月27~30日京津冀地区AOD进行反演研究,并与AERONET地基观测AOD数据进行了对比分析.结果表明,基于FY-4A数据及构建响应函数库,通过暗像元方法能较好的反演出京津冀地区气溶胶空间分布;AOD主要的高值区体现在京津冀中南部地区并向周边郊区逐渐降低,在AOD值较大时此特征较为明显;将反演值与同期AERONET地基观测数据对比验证,相关系数达到0.869,均方根误差为0.221,表明AOD反演值与观测值吻合较好,FY-4A卫星数据反演AOD具有一定可行性.     

基于FY-4A卫星数据反演气溶胶光学厚度及分析应用

风云四号A星（FY-4A）是我国新一代静止气象卫星,多通道扫描成像辐射计（AGRI）是风云四号静止气象卫星的主要载荷之一.为探究FY4A数据用于气溶胶光学厚度（AOD）反演的可行性,基于FY-4A/AGRI数据,利用暗像元算法对2019年2月23~26日及10月27~30日京津冀地区AOD进行反演研究,并与AERONET地基观测AOD数据进行了对比分析.结果表明,基于FY-4A数据及构建响应函数库,通过暗像元方法能较好的反演出京津冀地区气溶胶空间分布;AOD主要的高值区体现在京津冀中南部地区并向周边郊区逐渐降低,在AOD值较大时此特征较为明显;将反演值与同期AERONET地基观测数据对比验证,相关系数达到0.869,均方根误差为0.221,表明AOD反演值与观测值吻合较好,FY-4A卫星数据反演AOD具有一定可行性.     

重庆市交通扬尘尘源的鉴别

采用因子分析的方法解析重庆市城区交通干道上交通扬尘的尘源,结果表明该地区交通扬尘的主要来源是土壤、燃煤,汽车和治金源排放,其中土壤贡献了交通扬尘总量的大约一半,而另一半则来自其它人为活动。      

影响北仑区域能见度的因素研究

利用对北仑区域内的气溶胶散射系数、气溶胶浓度、黑炭浓度以及NO2浓度的监测和分析,对区域影响能见度的的因素进行了研究,研究结果表明,影响能见度的消光系数主要由气溶胶的散射、气溶胶的吸收,干洁大气的散射和气态污染物的吸收四项组成,且组成比例总体稳定,但是,不同空气质量级别和灰霾天与非灰霾天之间的消光系数值及组成差异较大;通过对气溶胶与光散射系数的拟合得到,两者存在较好的正相关性。     

某市气溶胶的分布特征研究

利用美国PC—2型气溶胶粒度分析仪,对淮南市的气溶胶现状进行厂流动监测,并研究其分布特征。结果表明,淮南市的气溶胶从西北向东南有明显的扩散趋势,最大浓度出现在早晨7～8时。大于1.0μm粒径的颗粒对气溶胶污染贡献较大。     

Infrared spectroscopic probing of dimethylamine clusters in an Ar matrix

Amines have many atmospheric sources and their clusters play an important role in aerosol nucleation processes. Clusters of a typical amine, dimethylamine (DMA), of different sizes were measured with matrix isolation IR (infrared) and NIR (near infrared) spectroscopy. The NIR vibrations are more separated and therefore it is easier to distinguish different sizes of clusters in this region. The DMA clusters, up to DMA tetramer, have been optimized using density functional methods, and the geometries, binding energies and thermodynamic properties of DMA clusters were obtained. The computed frequencies and intensities of NH-stretching vibrations in the DMA clusters were used to interpret the experimental spectra. We have identified the fundamental transitions of the bonded NH-stretching vibration and the first overtone transitions of the bonded and free NH-stretching vibration in the DMA clusters. Based on the changes in vibrational intensities during the annealing processes, the growth of clusters was clearly observed. The results of annealing processes indicate that DMA molecules tend to form larger clusters with lower energies under matrix temperatures, which is also supported by the calculated reaction energies of cluster formation.     

Analysis of the origin of peak aerosol optical depth in springtime over the Gulf of Tonkin

By aggregating MODIS(moderate-resolution imaging spectroradiometer) AOD(aerosol optical depth) and OMI(ozone monitoring instrument) UVAI(ultra violet aerosol index)datasets over 2010–2014, it was found that peak aerosol loading in seasonal variation occurred annually in spring over the Gulf of Tonkin(17–23°N, 105–110°E). The vertical structure of the aerosol extinction coefficient retrieved from the spaceborne lidar CALIOP(cloud-aerosol lidar with orthogonal polarization) showed that the springtime peak AOD could be attributed to an abrupt increase in aerosol loading between altitudes of 2 and 5 km.In contrast, aerosol loading in the low atmosphere(below 1 km) was only half of that in winter. Wind fields in the low and high atmosphere exhibited opposite transportation patterns in spring over the Gulf of Tonkin, implying different sources for each level. By comparing the emission inventory of anthropogenic sources with biomass burning, and analyzing the seasonal variation of the vertical structure of aerosols over the Northern Indo-China Peninsula(NIC), it was concluded that biomass burning emissions contributed to high aerosol loading in spring. The relatively high topography and the high surface temperature in spring made planetary boundary layer height greater than 3 km over NIC. In addition, small-scale cumulus convection frequently occurred, facilitating pollutant rising to over 3 km, which was a height favoring long-range transport. Thus, pollutants emitted from biomass burning over NIC in spring were raised to the high atmosphere, then experienced long-range transport, leading to the increase in aerosol loading at high altitudes over the Gulf of Tonkin during spring.     

MAX-DOAS observation in the midlatitude marine boundary layer: Influences of typhoon forced air mass

As a passive remote sensing technique, MAX-DOAS method was widely used to investigate the vertical profiles of aerosol and trace gases in the lower troposphere. However, the measurements for midlatitude marine boundary layer are rarely reported, especially during the storm weather system. In this study, the MAX-DOAS was used to retrieve the aerosol, HCHO and NO₂ vertical distribution at Huaniao Island of East China Sea in summer 2018, during which a strong tropical cyclone developed and passed through the measurement site. The observed aerosol optical depth (AOD), HCHO- and NO_2-VCDs (Vertical Column Density) were in the range of 0.19-0.97, (2.57-12.27) × 10¹⁵ molec/cm², (1.24-4.71) × 10¹⁵ molec/cm², which is much higher than remote ocean area due to the short distance to continent. The vertically resolved aerosol extinction coefficient (AEC), HCHO and NO₂ presented the decline trend with the increase of height. After the typhoon passing through, the distribution of high levels of aerosol and HCHO stretched to about 1 km and the abundances of the bottom layer were found as double higher than before, reaching 0.51 km⁻¹ and 2.44 ppbv, while NO₂ was still constrained within about 300 m with 2.59 ppbv in the bottom layer. The impacts of typhoon process forced air mass were also observed at the suburban site in Shanghai in view of both the aerosol extinction and chemical components. The different changes on air quality associated with typhoon and its mechanism in two different environments: coastal island and coastal city are worthy of further investigation as it frequent occurred in East Asia during summer and fall.     

重庆大气颗粒物与酸性降水关系研究

本文研究了重庆不同区域、不同季节、不同粒径的大气颗粒物的主要理化性能与酸性降水的关系,表明城区酸性细粒径颗粒物(IP、粒径<10μm)占 TSP 重量百分数为73％,大气颗粒物对酸性降水的缓冲能力较弱,通常冬(秋)季对降水酸度有一定贡献。     

Size-resolved carbonaceous components and water-soluble ions measurements of ambient aerosol in Beijing

A MOUDI-120 sampler was used in Beijing to collect multi-stage samples in the summer and winter of 2013 to 2015. Thirty-three sample sets were collected during the daytime,nighttime, and different pollution levels. The actual relative humidity in the impactors was calculated for the first time. The carbonaceous components(organic and elemental carbon,OC and EC, respectively) and water-soluble inorganic ions(Na~+, NH_4~+, K~+, Mg~(2+), Ca~(2+), Cl~-, NO_3~-,and SO_4~(2-)) were analyzed in each sample. The characteristics of the mass concentration distribution and charge balance were discussed. On the basis of relative humidity in the impactors, aerosols less than 1.0 μm were sampled under relatively dry conditions in most cases. The concentration levels for the chemical species were higher in the winter than in the summer. Three modes(condensation mode, droplet mode, and coarse mode) could be identified from the distributions of NH_4~+, NO_3~-, SO_4~(2-), Cl~-, K~+, OC and EC. The distribution characteristics for the pollution dissipation process were different from the pollution accumulation process. NO_3~-and NO_2~-contributed most of the negative electric charges in the stage below 0.1 μm. In the condensation mode, the cations were dominated by NH_4~+, which was sufficient to balance the anions. In the droplet mode of the heavily polluted samples,the ammonium was not sufficient to balance the anions. In the coarse mode, the positive electric charges were primarily composed of metal cations. The analyzed anions were not sufficient to neutralize the measured cations.     

MODIS遥感气溶胶光学厚度产品在地面能见距中的应用

利用气象站点能见距的历史资料和NASA的MOD1S卫星遥感手段获取10km＊10km分辨率的气溶胶光学厚度资料，建立二者之间的季节平均关系。得到了上海地区季节变化的气溶胶标高，并利用标高数据和气溶胶光学厚度的季节分布。反演出上海地区季节变化的区域能见距分布，研究近地层大气气溶胶与地面能见距的关系，分析上海市能见度时空分布特征，结果显示：上海城区在冬春季平均能见距较差，市区中心能见距在lOkm以下；低能见距中心分布明显。且主要分布在杨浦、桃浦、吴淞等工业区范围。     

MODIS遥感气溶胶光学厚度产品在地面能见距中的应用

利用气象站点能见距的历史资料和NASA的MODIS卫星遥感手段获取10km*10km分辨率的气溶胶光学厚度资料,建立二者之间的季节平均关系,得到了上海地区季节变化的气溶胶标高,并利用标高数据和气溶胶光学厚度的季节分布,反演出上海地区季节变化的区域能见距分布,研究近地层大气气溶胶与地面能见距的关系,分析上海市能见度时空分布特征,结果显示:上海城区在冬春季平均能见距较差,市区中心能见距在10km以下;低能见距中心分布明显,且主要分布在杨浦、桃浦、吴淞等工业区范围.     

浦东新区大气气溶胶中碳颗粒的分布规律

采用元素相关性分析方法，找出浦东新区大气气溶胶中碳颗粒的污染源，确证该区大气中碳颗粒主要来自煤的燃烧。同时初步找出浦东新区大气中碳颗粒污染的时空分布和粒径分布规律，为改善浦东 新区大气污染状况提供依据。     

自然通风对办公室内气溶胶的影响

办公室间歇开窗自然通风可降低空内颗粒物和微生物的浓度，用ＴＳＩ公司的气溶胶自动分析仪和ＦＡ－１型空气微生物采样器对样品测定结果表明，上午９：００室外大气颗粒物浓度高于室内，不宜开窗；１０：３０左右，室内颗粒物浓度增高，开窗自然通风效果好。     

南京市城区气溶胶粒度分布特征

以九段串级式撞击采样器对南京市气溶胶进行采样测定。经统计分析发现，气溶胶呈双峰分布，粒度分布规律明显，峰值粒径在0.37μm-0.65μm和4．3μm-5.6μm之间，气溶胶浓度季节变化显著，秋季＞夏秋，秋季颗粒物中细粒子质量百分比较夏季的多，两季质量中位位直径分别为6．5μm,4,4μm，说明与季节变化密切相关。     

2016年10～11月期间北京市大气颗粒物污染特征与传输规律

本研究采用气溶胶化学组分在线监测仪（ACSM）对北京地区2016年10月15日~11月15日期间非难熔性PM₁（NR-PM₁）化学组分进行实时连续在线观测,探讨了NR-PM₁化学组分的演变特征;运用潜在源贡献分析（PSCF）法和气象-空气质量模式（WRF-CAMx）识别了北京PM_2.5潜在污染源区和传输路径,揭示了PM_2.5净传输通量的垂直分布特征.结果表明,北京秋季NR-PM₁和PM_2.5质量浓度分别为（59.16±57.05）μg·m^-3和（89.82±66.66）μg·m^-3,其中NR-PM₁平均占PM_2.5的（70.31±22.28）%.整个观测期间,有机物（Org）、硝酸盐（NO₃^-）、硫酸盐（SO₄^2-）、铵盐（NH₄⁺）和氯化物（Chl）分别占NR-PM₁总质量浓度的（42.75±11.35）%、（21.27±7.72）%、（19.11±7.08）%、（12.19±2.64）%和（4.68±3.24）%,不同化学组分的日变化特征存在明显差异.对北京秋季NR-PM₁污染影响较大的潜在源区主要集中在河北南部、河南东北部及山东西部,重污染期间保定、北京南部及廊坊等城市对NR-PM₁贡献较大.WRF-CAMx模拟结果表明,PM_2.5总的净传输通量呈现出显著的垂直分布特征.整个观测期间,毗邻城市主要向北京输入PM_2.5,净通量最大出现在海拔600~1000 m;而重污染前期外来源输送PM_2.5主要位于高空,直到污染最严重的11月5日,PM_2.5转为近地面传输,说明高空和近地面传输是影响北京秋季PM_2.5重污染形成的重要因素.同时鉴别出了两种传输路径,即西南-东北方向（保定→北京→承德）和西北-东南方向（张家口→北京→廊坊北→天津）.