加入SOA示踪的深圳大气PM2.5受体模型源解析

为厘清包括二次有机气溶胶（SOA）在内的深圳市区PM_2.5各种一次和二次来源贡献,本文于2017年9月2日~2018年8月29日在深圳市大学城点位开展PM_2.5样品采集,并进行化学组分和水溶性有机物（WSOM）质谱测量,共获得162组有效数据.观测期间深圳市大气PM_2.5平均质量浓度为26μg/m³,在传统PMF源解析的基础上加入羧基离子碎片（CO₂⁺）作为SOA的示踪物,加入水溶性有机氧（WSOO）用于计算各因子O/C,验证有机物解析效果.结果表明,SOA可以被独立解析出,其O/C明显高于其他一次污染源中有机物;机动车、二次硫酸盐、二次硝酸盐、SOA为最主要的4个源,对PM_2.5质量浓度的贡献分别为25%、23%、17%和10%,船舶、地面扬尘、老化海盐、建筑尘、生物质燃烧、燃煤和工业贡献均在5%以内.各个源的变化特征表明,机动车、二次硫酸盐、二次硝酸盐、SOA等源贡献呈现冬高夏低的季节特征,与冬季季风条件下源自内陆的污染传输密切相关.污染天气时,二次硝酸盐和SOA的贡献增加相对最显著,因此NOx和挥发性有机物是减排的关键.     

华北地区沙尘天气垂直气溶胶直接辐射强迫

利用CALIOP数据和SBDART（Santa Barbara DISORT Atmospheric Radiative Transfer）辐射传输模式研究了2013~2016年华北地区8d沙尘天气气溶胶及其直接辐射强迫垂直分布特征,分析了气溶胶垂直分布和光学特性对直接辐射强迫的影响.结果表明,气溶胶集中分布在地表及以上3km范围,其中纯净沙尘型和污染沙尘型气溶胶位于上层,污染大陆型气溶胶和烟雾位于下层.大气层顶、地表和大气层的日均气溶胶直接辐射强迫分别是-38.41~-88.44,-74.03~-225.86,9.06~137.42W/m².0~8km高度范围气溶胶直接辐射强迫是负值,且随着高度的增加绝对值逐渐减小.气溶胶垂直分布对大气层顶、地表和大气层的直接辐射强迫影响较小,但对直接辐射强迫垂直分布影响较大,由气溶胶廓线差异造成的同一高度层气溶胶直接辐射强迫最大差值能达到31.18W/m².气溶胶光学厚度和单次散射反照率对直接辐射强迫影响明显.消光能力相同时,吸收性气溶胶对短波太阳光的衰减作用大于散射性气溶胶,后向散射比例大的气溶胶大于后向散射比例小的气溶胶.     

Characterization of atmospheric aerosol (PM10 and PM2.5) from a medium sized city in São Paulo state, Brazil

Air pollution causes deleterious effects on human health with aerosols being among the most polluting agents.The objective of this work is the characterization of the PM_(2.5) and PM_(10) aerosol mass in the atmosphere.The methods of analysis include WD-XRF and EDS.Data were correlated with meteorological information and air mass trajectories(model HYSPLIT)by multivariate analysis.A morphological structural analysis was also carried out to identify the probable sources of atmospheric aerosols in the city of Sao Jose do Rio Preto,Brazil.The mean mass concentration values obtained were 24.54 μg/m~3 for PM_(10),above the WHO annual standard value of 20 μg/m~3 and 10.88 μg/m~3 for PM_(2.5) whose WHO recommended limit is10 μg/m~3.WD-XRF analysis of the samples revealed Si and Al as major components of the coarse fraction.In the fine fraction,the major elements were Al and S.The SEM-FEG characterization allowed identifying the morphology of the particles in agglomerates,ellipsoids and filaments in the PM_(10),besides spherical in the PM_(2.5).The analysis by EDS corroborated WD-XRF results,identifying the crustal elements,aluminosilicates and elements of anthropogenic origin in the coarse fraction.For the fine fraction crustal elements were also identified;aluminosilicates,black carbon and spherical particles(C and O) originating from combustion processes were predominant.The use of multivariate analysis to correlate air mass trajectories with the results of the morpho-structural characterization of the particulate matter allowed confirmation of the complex composition of the particles resulting from the combination of both local and long-distance sources.     

Aerosol optical properties under different pollution levels in the Pearl River Delta (PRD) region of China

To clarify the aerosol hygroscopic growth and optical properties of the Pearl River Delta(PRD)region,integrated observations were conducted in Heshan City of Guangdong Province from October 19 to November 17,2014.The concentrations and chemical compositions of PM_(2.5),aerosol optical properties and meteorological parameters were measured.The mean value of PM_(2.5) increased from less than 35(excellent) to 35-75 μg/m~3(good) and then to greater than 75 μg/m~3(pollution),corresponding to mean PM_(2.5) values of 24.9,51.2,and 93.3 μg/m~3,respectively.The aerosol scattering hygroscopic growth factor(f(RH = 80%)) values were 2.0,2.12,and 2.18 for the excellent,good,and pollution levels,respectively.The atmospheric extinction coefficient(σext)and the absorption coefficient of aerosols(σ_(ap)) increased,and the single scattering albedo(SSA)decreased from the excellent to the pollution levels.For different air mass sources,under excellent and good levels,the land air mass from northern Heshan had lower f(RH) and σ_(sp) values.In addition,the mixed aerosol from the sea and coastal cities had lower f(RH) and showed that the local sources of coastal cities have higher scattering characteristics in pollution periods.     

2006-2017年四川盆地MODIS气溶胶光学厚度时空变化特征

四川盆地地形复杂、气候特殊,是我国颗粒物污染高发地.为探究四川盆地气溶胶分布和周期变化特征,深入认识气溶胶污染特性及其气候效应,结合卫星遥感探测方法,利用2006-2017年MODIS C006 3 km AOD（气溶胶光学厚度）产品,分析了四川盆地AOD的时空特征.结果表明:①MODIS AOD（MODIS数据反演的气溶胶光学厚度）与太阳光度计CE318观测的AOD、ρ（PM_2.5）、ρ（PM₁₀）线性相关系数分别为0.78、0.77、0.75,表明MODIS C006 3 km AOD产品适用于四川盆地颗粒物污染研究.②四川盆地AOD平均值范围为0.1~1.3,其中,成都平原和四川盆地东南部地区是AOD高值（AOD值>1.0）中心,四川盆地周边高海拔区AOD均小于0.3.③2006-2017年AOD年均值范围为0~2.5,整体呈"倒N型"曲线下降,其峰值和谷值分别出现在2013年和2017年;2013年AOD大于1.0的区域占四川盆地的34.1%,是12 a中颗粒物污染最重的一年;2017年AOD小于0.3的面积占57.1%.④AOD季节性变化呈春季最大、夏季次之、秋季最小的特征.⑤AOD月变化呈"双峰型"波动特征,AOD月均值范围为0~2.5,其中,2-5月AOD月均值均大于0.7,8月AOD月均值为0.6,11-12月AOD月均值均小于0.5.研究显示,四川盆地颗粒物污染防治应以成都平原城市群和四川省南部城市群为主,应重点控制细颗粒物排放,合理安排工业企业的周期性生产强度.      

Effect of NOx and SO2 on the photooxidation of methylglyoxal: Implications in secondary aerosol formation

Methylglyoxal(CH_3COCHO,MG),which is one of the most abundant α-dicarbonyl compounds in the atmosphere,has been reported as a major source of secondary organic aerosol(SOA).In this work,the reaction of MG with hydroxyl radicals was studied in a 500 L smog chamber at(293±3) K,atmospheric pressure,(18±2)% relative humidity,and under different NOx and SO_2.Particle size distribution was measured by using a scanning mobility particle sizer(SMPS) and the results showed that the addition of SO_2 can promote SOA formation,while different NOx concentrations have different influences on SOA production.High NOx suppressed the SOA formation,whereas the particle mass concentration,particle number concentration and particle geometric mean diameter increased with the increasing NOx concentration at low NOx concentration in the presence of SO_2.In addition,the products of the OH-initiated oxidation of MG and the functional groups of the particle phase in the MG/OH/SO_2 and MG/OH/NOx/SO_2 reaction systems were detected by gas chromatography mass spectrometry(GC-MS) and attenuated total reflection fourier transformed infrared spectroscopy(ATR-FTIR) analysis.Two products,glyoxylic acid and oxalic acid,were detected by GC-MS.The mechanism of the reaction of MG and OH radicals that follows two main pathways,H atom abstraction and hydration,is proposed.Evidence is provided for the formation of organic nitrates and organic sulfate in particle phase from IR spectra.Incorporation of NOx and SO_2 influence suggested that SOA formation from anthropogenic hydrocarbons may be more efficient in polluted environment.     

基于卫星遥感气溶胶产品评估体系的气溶胶时空分布及变化趋势表征

卫星遥感气溶胶虽然空间覆盖度高,但不同产品数据在准确性和适用性上存在显著差异.为了能够科学定量的衡量各个产品的优劣,选择最合适的气溶胶产品,该研究以数学统计为基础,提出了一种卫星遥感气溶胶产品评估体系,并依此确定了全球6个人口密集地区的最优卫星数据集,在此基础上开展了近10年的（2009—2018）气溶胶时空变化分析.结果表明暗像元算法在植被覆盖度高的地区表现最好,深蓝算法在亮地表的沙漠干旱地区更占优势,而暗像元-深蓝融合算法在土地类型复杂且气溶胶来源多变时得以突出.人口密集的6个区域中,除了区域A和区域B,其它地区的大气污染水平整体偏高.其中,A、B、E的气溶胶负荷呈下降变化,区域F基本不变,其余区域上升变化.评估体系的建立为气溶胶遥感产品的选取提供了新的衡量方法,且该文关于气溶胶时空分布及变化的分析可以为区域性气溶胶研究提供一定的参考价值.     

东南亚生物质燃烧输送影响我国西南气溶胶辐射特性研究

利用2013年地基CE-318太阳光度计观测数据,结合中分辨率成像光谱仪（MODIS）遥感产品和HYSPLIT后向轨迹分析,研究了一次东南亚生物质燃烧污染长距离输送至中国西南昆明站点过程（2013年4月5~8日）中,气溶胶光学特性和辐射特性的变化及其可能来源.结果表明,此次污染过程期间,我国西南地区生物质燃烧活动较少,而中南半岛地区生物质燃烧活动显著.4月5~7日,昆明站点气溶胶光学厚度（AOD）升高,消光波长指数（EAE）和吸收波长指数（AAE）均增大.此外,依据EAE和AAE分类方法,5~6日昆明站点以城市工业气溶胶为主,7~8日以生物质燃烧气溶胶为主,其细模态峰值半径（0.11μm）小于5~6日（0.15μm）,7日细模态粒子体积浓度峰值（约为0.16μm³/μm²）是5日的2倍.气溶胶直接辐射强迫（ARF）日变化结果表明4月7日气溶胶对地表的降温效应达到最大,对大气的加热作用最强.气溶胶直接辐射强迫效率值（ARFE）的变化表明生物质燃烧气溶胶对大气顶的降温作用减弱.MODIS遥感以及HYSPLIT模式后向轨迹表明,此次昆明站点生物质燃烧气溶胶主要来源于东南亚地区（主要是印度北部、印缅北部和不丹地区）.     

近14年西北地区甲醛柱浓度的时空变化研究

基于臭氧监测仪（OMI）卫星反演数据,对2005~2018年西北4省区域大气甲醛柱浓度数据进行提取及分析,探讨其时空变化特征及影响因素.结果表明：在时间变化上,14a甲醛柱浓度整体呈先上升后下降的波动变化趋势,夏秋季显著高于冬春季,且冬季均值略高于春季.在空间分布上,甲醛柱浓度自西向东、自北向南逐渐升高,高值区集中于陕西和甘肃东南部及青海西南部;低值区集中于宁夏、青海和甘肃的西北部;稳定性呈现出东部分散、西部集聚、差异显著的分布格局.影响甲醛柱浓度变化的因素包括自然和人为因素,自然因素中,甲醛柱浓度受地形影响显著,与风向、气温均呈现显著正相关;人为因素中,甲醛柱浓度与人口密度、地区生产总值、工业废气排放量及建筑房屋竣工面积均表现出正相关关系,与工业废气排放量的相关度最高.大气中甲醛分子与气溶胶粒子二者间呈显著正相关关系,这进一步说明甲醛浓度受到了诸多因素的综合影响,但气溶胶粒子、气温及工业废气的排放是主导因素.     

NOx存在条件下相对湿度对甲苯氧化产物的影响

利用流动管反应器模拟甲苯与氧化剂×OH在NO_x存在条件下的反应,定量测定了不同相对湿度条件下（17.5%、35%、50%、70%）反应生成的部分气相产物和颗粒相产物,计算了不同相中产物产率,测量了不同相对湿度下的颗粒相有机碳（OC）产率,推导了相对湿度对甲苯氧化反应的影响机制.结果表明,相对湿度不仅对甲苯与×OH反应途径比例有影响,还对产物的产率及氧化程度有影响.