交通限行对细颗粒物浓度及其谱分布的影响

采用电迁移率粒径谱仪SMPS 3936对颗粒物数浓度及其谱分布进行了实时监测,对2013年兰州市国际马拉松赛交通管制期间细颗粒物浓度及其谱分布特征开展研究,并通过多元对数正态分布拟合和主成分分析方法分别对数浓度谱特征及其影响因素进行了分析,以阐明2013年兰州国际马拉松赛期间交通管制对细颗粒物浓度及其谱特征的影响。气象条件相似的交通限行期间,交通限行日50~100 nm,100~200 nm和200~500 nm粒径段颗粒物数浓度均较正常周六有所降低,特别是50~200nm粒径段颗粒物表现最为显著,在此期间,交通限行日50~100 nm和100~200 nm粒径段平均颗粒物数浓度分别为2567.5±807.4 cm-3和1567.8±193.8 cm-3,分别较正常周六相应时段低60.2%和67.2%。交通限行对颗粒物数浓度的影响主要集中在107 nm为峰值粒径的积聚模态附近,而气象条件对10~300 nm粒径段颗粒物数浓度均有较显著的影响,最大影响在80 nm附近。     

关中颗粒物粒径谱特征及其气象影响因子分析

利用西安泾河和长安的气象观测资料、陕西秦岭大气科学试验基地气溶胶粒子谱观测资料及西安市环境保护局颗粒物质量浓度观测资料,分析了气象条件对关中颗粒物粒径谱的影响,结果表明:关中特殊的地形影响和严重的颗粒物污染是霾易发的主要原因;混合层高度与PM_(2.5)质量浓度具有较明显的负相关关系,秋、冬季混合层高度高有利于颗粒物污染的扩散。不同方向上风速变化对颗粒物浓度的影响体现了西北气流对关中颗粒物污染的扩散作用和偏东气流对颗粒物污染的输送。高相对湿度有利于稳定层结的维持和污染物集聚,当相对湿度≤80%时,粒径在150nm～1.0μm的粒子的数浓度,随着相对湿度的增大明显增加,对降低能见度、形成雾-霾有重要作用。不同粒径段粒子的数浓度随相对湿度的变化不同,对能见度的影响也不同;相对湿度越大,湿度对降低能见度的贡献越大。     

南京地区气溶胶谱分布的湿度相关性分析和等效复折射率预测

通过实验收集大气颗粒物，对南京地区大气气溶胶谱分布进行了描述，对气溶胶分布与相对湿度的相关性进行了探讨。建立了南京地区7—11月气溶胶化学组分的月平均模型，得出气溶胶等效复折射率的预测方法。结果表明：南京地区的大气气溶胶颗粒物，峰值粒径在80~100 nm范围，属于典型的城市型气溶胶。数浓度与相对湿度的相关性与季节和粒径大小有关，在6—9月，相对湿度与细粒子数浓度呈负相关，与粗粒子呈正相关，在10—11月相反，且易受极端天气影响。建立的干气溶胶等效复折射率月平均模型，结合湿度修正模型得到某一日的复折射率，与AERONET站点数据进行了对比，结果较为一致，误差范围在0~0.03。     

南京一次重霾天气纳米气溶胶观测研究

为加深对南京地区重霾天气过程纳米尺度气溶胶物理特征的了解,对2017年12月21-25日的一次重霾天气过程进行了综合探测,利用宽范围粒径谱仪观测了此次过程中10～1000 nm颗粒物数浓度,并结合能见度等气象要素,对重霾期间纳米气溶胶谱分布进行了分析.结果 表明:此次霾重污染过程出现在低温、高湿、气压上升期间;与非重污...     

南京市夏季城市不同功能区气溶胶污染特征

利用ＷＰＳ（宽范围颗粒粒径谱仪）、Ａｎｄｅｒｓｏｎ Ⅱ型９级撞击采样器测量了２００８年夏季典型日南京钟山风景区、鼓楼商业区与江北工业区大气气溶胶数浓度谱分布和质量浓度,分析了城市不同功能区气溶胶粒子的分布特征．结果表明：各功能区大气颗粒物浓度均比较高,达到１０４ｃｍ－３,数浓度谱均为单峰型,峰值集中在００１～００４μｍ;其中气溶胶粒子数浓度主要集中在００１～０２μｍ粒径范围内,其日变化受汽车尾气排放、混合层高度变化的影响较大,且呈现明显的双峰型;粒径为００１～０１μｍ的超细粒子对总数粒子贡献较大,鼓楼为９３２８％,江北为８１６６％,钟山为６６５２％;细粒子（粒径＜１１μｍ）与ＴＳＰ质量浓度的比值钟山为９２％,鼓楼３３７７％, 江北２４９８％;质量浓度主要为粗粒子（粒径≥１１μｍ）贡献,但是鼓楼与江北的细粒子的贡献也非常大,说明这两个功能区的细粒子的污染值得关注;数浓度和相对湿度（ＲＨ）有密切联系,当ＲＨ＜７５％时其峰值随着相对湿度的增大而增大,当ＲＨ＞７５％时其峰值随着相对湿度的增大而减少,并且相对湿度对细粒子的影响要大于对大粒子的影响．     

安徽省雾、霾、晴空天气的气象条件对比分析

使用2008~2012年逐日地面观测资料,揭示了安徽不同地区雾、霾、晴空天气气象条件的差异,指出不同地区要根据本地特点建立雾、霾预报指标和预报方法。3类天气差异最大的地面气象要素是能见度和相对湿度。根据3种天气前一日和当日能见度和相对湿度分布特征,全省站点可以分为3类:1)从雾、霾到晴空,能见度递增、相对湿度递减,且差异显著,如合肥站;2)雾、霾天的能见度和相对湿度均很接近,但与晴空天差别较大,如阜阳站;3)能见度在雾、霾天无明显差别,但相对湿度在雾、霾天差异显著,如安庆站。地级市测站雾后即霾的可能性较大(大于50%),县城测站雾后即霾的可能性较低(低于25%)。垂直方向,雾时相对湿度随高度下降很快,850 h Pa中位值已降到20%(安庆)和45%(阜阳)以下,霾时相对湿度随高度下降缓慢,850 h Pa中位值仍在60%左右;另外,霾天边界层中上部风切变较小,雾天和晴空天边界层中上部都存在较大的风切变。     

南京霾天气的特征分析和影响因子初探

根据南京气象观测站2004年1月—2008年7月逐日观测资料,南京市环境质量监测点2004年1月—2007年12月SO2、NO2、PM10的逐日实测资料,对南京市霾天气的气象要素特征及其成因进行了初步分析。结果表明:(1)南京霾现象多发生在中午前后,11时出现的次数最多;春秋冬季霾天气出现时次多,夏季少。(2)南京霾天气时能见度多在4~8 km范围内;静小风,风速主要在1~3 m/s,偏东风时霾天气发生较多;相对湿度在40%~70%间有利于霾天气出现,尤以50%~60%时出现概率最高。(3)大气颗粒物(特别是细颗粒物)污染加剧,很可能是南京霾天气频发的一个重要原因。     

北京2013年1月严重霾天气过程的气象成因分析

利用常规观测资料、地面自动站资料及NCEP 1°×1°分析资料,结合边界层散度场的诊断分析,探讨了北京2013年1月严重霾天气过程的环流特征和气象成因。主要结论如下: 1)500 hPa为偏西气流,冷空气活动弱,无明显冷平流,对流层低层850 hPa及其以下风速小、冷空气活动偏弱,是霾天气的显著特征。2)边界层存在逆温和大气层结稳定是霾发生的另一重要条件,逆温层不仅可出现在边界层,有时也出现在对流层低层850 hPa 附近。3)边界层存在弱辐合中心是霾形成的重要条件,特别是在区域性污染的情况下,边界层辐合可使霾因区域性污染物的输送汇聚而加重。4)偏东风对霾形成和加重具有重要作用,主要表现为风速一般较小,在边界层形成暖平流结构,易形成逆温,增加边界层相对湿度和维持边界层辐合,配合北京西部山地特殊地形,使污染物积累,最终通过增大污染物浓度及增大边界层相对湿度,造成大气水平能见度严重降低。5）1月10—14日霾天气过程主要是在边界层有弱辐合而相对湿度较低的条件下形成的,而27—31日过程主要发生在边界层相对湿度较高的条件下。     

华东高海拔地区夏季气溶胶数浓度及谱分布特征

利用2014年7月黄山光明顶观测获得的气溶胶数浓度、气溶胶数谱数据,对黄山夏季气溶胶数浓度及谱分布特征进行分析,并在此基础上对气溶胶数谱进行了对数正态分布拟合。研究结果表明:黄山夏季气溶胶平均数浓度约为3 518.27 cm~(-3),主要集中在爱根核模态;气溶胶平均数浓度日变化呈双峰分布,峰值浓度的出现伴随着小粒子的增多。气溶胶数浓度与相对湿度和风速成负相关,高浓度的气溶胶多出现在较弱的东南风时;积聚模态气溶胶数浓度受风向影响显著。不同气团背景下气溶胶数谱差异集中在小于100 nm和500~1 000 nm粒径范围。爱根核模态气溶胶在高湿的西南气团影响下数浓度最低、谱较窄,而高温、低湿的东南气团对应的气溶胶数浓度最高、谱最宽,北方气团对应的气溶胶数浓度和谱宽居中;500~1 000 nm粒径范围气溶胶数谱分布特征与之相反。不同背景的气溶胶数谱和体积谱均可采用爱根模态、积聚模态1和积聚模态2三个模态进行对数正态分布拟合,但不同气团背景下的各模态谱型参数差异较大。     

“13·12”西安重污染气象条件及影响因素

使用高分辨监测资料对2013年12月18—25日西安严重污染天气气象条件及影响因素进行分析。结果表明:严重污染期间,亚洲大陆中高纬度500 hPa呈一槽一脊经向环流型,陕西处于地面冷高压南部均压场控制下。空气质量转好时,高空锋区明显增强,地面冷锋快速东移、南压,边界层高度增大,近地层集聚污染物显著抬升。严重污染与非污染时段气象条件差异明显。除接地逆温外,近地层不同高度存在悬浮逆温,相对湿度呈湿-干-湿垂直分布,温湿条件有利于污染加强。严重污染属于以湿霾为主的重度霾天气,日平均能见度小于1.5 km,边界层高度小于0.7 km,郊区湿霾每日持续时间平均比市区长约5 h。严重污染期间,细颗粒物浓度远高于粗颗粒物,随时间增加趋势明显。颗粒物平均浓度在午后出现峰值,可能与边界层高度偏低、关中盆地地形因素密切相关,本地地面风场日变化对污染有加重效应。     

Incorporation of aerosol particles between 25 and 850 nm into cloud elements: measurements with a new complementary sampling system

The interpretation of the physico-chemical processes in clouds is facilitated by segregating in situ cloud elements from their carrier gas and small particles (interstitial aerosol). Thus, the present study focuses on the quantitative phase segregation of interstitial air from cloud phase by two complementary samplers with microphysical on-line analysis of the separated phases. An improved counterflow virtual impactor (CVI) was developed for the collection and subsequent evaporation of the condensed phase, releasing dissolved gaseous material and residual particles. This sampler operates in the size range of few micrometers up to 50 μm in cloud element diameter and is matched by an interstitial Round Jet Impactor sampling the gas phase with interstitial particles. Calibrations of both samplers verified the calculated cut sizes D₅₀ of 4, 5, and 6 μm and quantified the slope of the collection efficiency curves. Until this study no direct CVI measurements of the residual particle sizes far below the diameter of 0.1 μm were available. For the first time a CVI was connected to a Differential Mobility Particle Sizer (DMPS) scanning between 25 nm and 850 nm, thus, including the entire Aitken mode in the residual size analysis. Cloud studies on the Puy de Dôme, France, revealed residual particle sizes including Aitken mode (diameter D<100 nm) and accumulation mode (D>100 nm). A major feature of the CVI data is expressed by the fact that despite incomplete incorporation of accumulation mode particles in cloud elements there are contributions of particles with diameters smaller than 0.1 μm to the number of residual particles. Cloud entrainment from height levels above the maximum supersaturation as wells as the size-dependent chemical composition of the aerosol population most likely produced the S-shaped size-dependent partitioning of residual particles. Compared to earlier studies the 50% partitioning diameters dropped significantly below 100 nm to roughly 70 nm.     

A closure study of sub-micrometer aerosol particle hygroscopic behaviour

The hygroscopic properties of sub-micrometer aerosol particles were studied in connection with a ground-based cloud experiment at Great Dun Fell, in northern England in 1995. Hygroscopic diameter growth factors were measured with a Tandem Differential Mobility Analyser (TDMA) for dry particle diameters between 35 and 265 nm at one of the sites upwind of the orographic cloud. An external mixture consisting of three groups of particles, each with different hygroscopic properties, was observed. These particle groups were denoted less-hygroscopic, more-hygroscopic and sea spray particles and had average diameter growth factors of 1.11–1.15, 1.38–1.69 and 2.08–2.21 respectively when taken from a dry state to a relative humidity of 90%. Average growth factors increased with dry particle size. A bimodal hygroscopic behaviour was observed for 74–87% of the cases depending on particle size. Parallel measurements of dry sub-micrometer particle number size distributions were performed with a Differential Mobility Particle Sizer (DMPS). The inorganic ion aerosol composition was determined by means of ion chromatography analysis of samples collected with Berner-type low pressure cascade impactors at ambient conditions. The number of ions collected on each impactor stage was predicted from the size distribution and hygroscopic growth data by means of a model of hygroscopic behaviour assuming that only the inorganic substances interacted with the ambient water vapour. The predicted ion number concentration was compared with the actual number of all positive and negative ions collected on the various impactor stages. For the impactor stage which collected particles with aerodynamic diameters between 0.17–0.53 μm at ambient relative humidity, and for which all pertinent data was available for the hygroscopic closure study, the predicted ion concentrations agreed with the measured values within the combined measurement and model uncertainties for all cases but one. For this impactor sampling occasion, the predicted ion concentration was significantly higher than the measured. The air mass in which this sample was taken had undergone extensive photochemical activity which had probably produced hygroscopically active material other than inorganic ions, such as organic oxygenated substances.     

MEASUREMENTS OF PARTICLE NUMBER SIZE DISTRIBUTIONS AND NEW PARTICLE FORMATION EVENTS DURING WINTER IN THE PEARL RIVER DELTA REGION, CHINA

Particle number size distribution(PNSD) between 10 nm and 20 μm were measured in the Pearl River Delta(PRD) region in winter 2011.The average particle number concentration of the nucleation mode(10-20 nm),Aitken mode(20-100 nm),accumulation mode(100 nm-1μm) and coarse mode(1-20 μm) particles were 1 552,7 470,4 012,and 19 cm-3,respectively.The volume concentration of accumulation mode particles with peak at 300 nm accounted for over 70% of the total volume concentration.Diurnal variations and dependencies on meteorological parameters of PNSD were investigated.The diurnal variation of nucleation mode particles was mainly influenced by new particle formation events,while the diurnal variation of Aitken mode particles correlated to the traffic emission and the growth process of nucleation mode particles.When the PRD region was controlled by a cold high pressure,conditions of low relative humidity,high wind speed and strong radiation are favorable for the occurrence of new particle formation(NPF) events.The frequency of occurrence of NPF events was 21.3% during the whole measurement period.Parameters describing NPF events,including growth rate(GR) and source rate of condensable vapor(Q),were slightly larger than those in previous literature.This suggests that intense photochemical and biological activities may be the source of condensable vapor for particle growth,even during winter in the PRD.     

Small-particle concentration fluctuations at a coastal site

Aerosol size spectra (d=10 nm–10 μm) were measured with an electrical aerosol spectrometer (EAS) at Mace Head on the west coast of Ireland. Several small aerosol particle (diameter 10–32 nm) concentration bursts were observed during the measurement period. Relationships between the events, air mass trajectories, tide height, and meteorological parameters are examined. Series of bursts were observed when a spectral transformation due to subsequent particle growth from 10 to 56–100 nm can be identified in an Eulerian experiment. Particle growth rates of between 1 and 3 nm/h were determined. These bursts appear in cold and comparatively clean arctic or polar air masses with temperature and relative humidity fluctuations, and do not correlate with low tide in some cases. These episodes, similar to those frequently found in the continental boundary layer, are thought to occur over a wide area and, for clear detection, require stable airflow for a few days. Elevated small-particle concentration events are more common during low tide or shortly after, and are typically associated with low wind speeds. Here, the increased shore exposure during low tide is thought to influence the nucleation and the subsequent growth of these aerosol particles. The occurrences of the bursts are found to depend on local wind direction. The highest d=10–32 nm particle concentrations appeared for wind sectors furthest from the tidal regions when the wind direction was 150–160°(south-easterly). Most of the events occurred during daytime when solar irradiation is most intense.     

A multifunctional HTDMA system with a robust temperature control

The hygroscopicity of atmospheric aerosols significantly influences their size distribution, cloud condensation nuclei ability, atmospheric residence time, and climate forcing. In order to investigate the hygroscopic behavior of aerosol particles and serious haze in China, a Hygroscopic Tandem Differential Mobility Analyzers (HTDMA) system was designed and constructed at Fudan University. It can function as a scanning mobility particle sizing system to measure particle size distribution in the range of 20--1000 nm in diameter, as well as a hygroscopicity analyzer for aerosol particles with diameters between 20--400 nm in the range of 20%--90% RH (relative humidity). It can also measure the effect of uptake of inorganic acids or semi-VOCs on the hygroscopic behavior of aerosols, such as typical inorganic salts in atmospheric dust or their mixtures. The performance tests show that the system measured particle size of the standard polystyrene latex spheres (PSLs) is 197 nm, which is in excellent agreement with the certified diameter D=199±6 nm, as well as a standard deviation of the repeated runs SD=8.9x10^-4. In addition, the measured hygroscopic growth factors of the model compounds, (NH₄)₂SO₄ and NaNO₃, agree with the Kohler theoretical curves. The results indicate that the HTDMA system is an excellent and powerful tool for studying the hygroscopic behavior of submicron aerosols and meets the demand required for laboratory research and fieldwork on atmospheric aerosols in China.     

Physical characterization of aerosol particles during nucleation events

Particle concentrations and size distributions have been measured from different heights inside and above a boreal forest during three BIOFOR campaigns (14 April–22 May 1998, 27 July–21 August 1998 and 20 March–24 April 1999) in Hyytiälä, Finland. Typically, the shape of the background distribution inside the forest exhibited 2 dominant modes: a fine or Aitken mode with a geometric number mean diameter of 44 nm and a mean concentration of 1160 cm⁻³ and an accumulation mode with mean diameter of 154 nm and a mean concentration of 830 cm⁻³. A coarse mode was also present, extending up to sizes of 20 μm having a number concentration of 1.2 cm⁻³, volume mean diameter of 2.0 μm and a geometric standard deviation of 1.9. Aerosol humidity was lower than 50% during the measurements. Particle production was observed on many days, typically occurring in the late morning. Under these periods of new particle production, a nucleation mode was observed to form at diameter of the order of 3 nm and, on most occasions, this mode was observed to grow into Aitken mode sizes over the course of a day. Total concentrations ranged from 410–45 000 cm⁻³, the highest concentrations occurring on particle production days. A clear gradient was observed between particle concentrations encountered below the forest canopy and those above, with significantly lower concentrations occurring within the canopy. Above the canopy, a slight gradient was observed between 18 m and 67 m, with at maximum 5% higher concentration observed at 67 m during the strongest concentration increases.     

Condensation particle counting below 2 nm seed particle diameter and the transition from heterogeneous to homogeneous nucleation

Particle detection by condensation particle counters (CPCs) is ultimately limited by the onset of homogeneous nucleation. At vapour supersaturations around the homogeneous nucleation limit the diameter of critical clusters is typically about 2 nm. It is widely assumed that only particles larger than critical clusters can be activated by vapour condensation and the general detection limit of CPCs is therefore currently accepted to be around 2 nm particle diameter. Using an expansion type CPC with n-propanol as working fluid we investigated the transition from heterogeneous to homogeneous nucleation, clearly showing that particles are activated much before the onset of homogeneous nucleation, even at particle diameters as small as 1.4 nm. For particle diameters below 2 nm we have usually found condensation particle counting to be influenced by the simultaneous presence of ions as generated in a bipolar diffusion charger. In this paper we illustrate how the presence of ions influences particle number concentration measurement and how ions can be removed in order to obtain accurate seed particle number concentrations for particle diameters down to 1 nm.     

Condensation particle counting below 2 nm seed particle diameter and the transition from heterogeneous to homogeneous nucleation

Particle detection by condensation particle counters (CPCs) is ultimately limited by the onset of homogeneous nucleation. At vapour supersaturations around the homogeneous nucleation limit the diameter of critical clusters is typically about 2 nm. It is widely assumed that only particles larger than critical clusters can be activated by vapour condensation and the general detection limit of CPCs is therefore currently accepted to be around 2 nm particle diameter. Using an expansion type CPC with n-propanol as working fluid we investigated the transition from heterogeneous to homogeneous nucleation, clearly showing that particles are activated much before the onset of homogeneous nucleation, even at particle diameters as small as 1.4 nm. For particle diameters below 2 nm we have usually found condensation particle counting to be influenced by the simultaneous presence of ions as generated in a bipolar diffusion charger. In this paper we illustrate how the presence of ions influences particle number concentration measurement and how ions can be removed in order to obtain accurate seed particle number concentrations for particle diameters down to 1 nm.