一次霾天气条件下石家庄上空大气气溶胶数浓度的飞行探测与特征分析

利用2010年8月30日河北省石家庄一次霾天气条件下的气溶胶飞行探测资料,分析了石家庄地区上空658—6933 m高度范围内大气气溶胶粒子平均数浓度、平均直径的垂直分布特征和9个水平飞行高度上的谱分布特征。结果表明:轻度霾天气条件下的气溶胶平均数浓度为325个/cm3,平均直径为0.169μm。在约1000 m高度以下,气溶胶平均数浓度随高度的增加呈线性减少趋势。粒径也随高度增加而减小,由0.187μm减小至0.164μm。1000 m高度以上,气溶胶平均数浓度随高度减少趋势变缓,粒子平均直径在0.167~0.171μm范围内波动。9个不同高度上的谱分布都呈单峰型,随着高度增加,谱宽变小,峰值向小尺度方向移动。后向轨迹计算分析表明:污染气团的远距离输送可能是导致大气1500 m高度层气溶胶数浓度突增的原因。     

石家庄地区2005年秋季污染气溶胶飞机观测资料分析

利用河北省2005年10月份的3次气溶胶飞机观测资料和宏观天气资料,综合分析石家庄地区不同天气条件下气溶胶的垂直分布和尺度谱分布特征。分析结果表明:气溶胶浓度的分布与大气环境情况密切相关。气溶胶数浓度最大值的变化范围是103~104cm-3,平均数浓度为103cm-3,粒子平均直径为0.120~0.150μm;21日近地面有霾,相对湿度为58%,近地面气溶胶浓度较17和29日略低,但粒子平均直径(0.165μm)比其余两次要大,可见相对湿度较大,大气中水汽含量较多,有利于小粒子凝结水汽,使粒子直径增大;逆温层结下,粒子在逆温层下累积,无逆温时数浓度最大值出现在近地面附近。气溶胶粒子谱呈单峰分布。     

天津大气气溶胶化学组分的粒径分布和垂直分布

2006年8月在天津气象铁塔的10、120、220 m 3个不同高度.利用Andersen分级采样器同步进行大气气溶胶采样,样品用离子色谱和电感耦合等离子体质谱仪进行分析.结果表明,K元素主要集中在细粒子,Mg、Ca、Al、Fe元素主要集中在粗粒子,Na元素则具有双峰结构;总离子浓度随着高度的升高有增加的趋势,SO42-、N3-、NH4+、Ca2+是最主要的水溶性尤机离子;二次源是水溶性离子重要的贡献源.NO3-、SO42-、NH4+随着高度升高,浓度有向小粒径集中的趋势;各层气溶胶阴阳离子平衡值小于1,表明气溶胶偏碱性,与天津地处北方,土壤偏碱性,且非采暖期地面扬尘是主要的气溶胶来源有关;各层NO3-/SO42-平均值为0.48,表明非采暖期固定排放源(燃煤)仍然是天津大气细粒子中水溶性离子的主要来源.     

南京气溶胶水溶性离子粒径分布及其随高度的变化

2009年1月对南京市河西生活区距地面1．5、54和80m3处同步进行了大气颗粒物采样,并用离子色谱对样品进行了分析。结果显示,随着高度的增加,PM10和PM2.1的质量浓度逐渐降低,而总离子浓度随高度增加而增大。气溶胶中最主要的3种水溶性离子分别为N03、SO4 2-、Ca2＋,且3个高度的NO3-与SO4 2-浓度之比均大于1,表明该生活区移动排放源已经成为大气气溶胶离子的主要来源。3个高度处各离子粒径分布规律为：SO4 2-、NO3-、K＋在0．43-1．1um出现峰值;Ca2＋、Mg2＋、NO2-在4．7～5．8um出现峰值;Na＋、Cl-、F-在0．43～1．1um和4．7～5．8um出现双峰。     

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.     

香河地区亚微米气溶胶粒子尺度谱分布特征

为了解香河地区气溶胶尺度谱的基本特征,自2012年5月起,利用扫描电迁移率粒径谱仪(SMPS)对河北香河地区的亚微米(13.8~723.4 nm)气溶胶尺度谱分布进行了近2 a的测量。基于该数据集,分析了气溶胶尺度谱的季节变化和日变化特征及气象要素对气溶胶浓度的影响。结果发现,观测期间埃根核模态(20.0~100.0 nm)、积聚模态(100.0~723.4 nm),以及总的气溶胶数浓度、表面积浓度和体积浓度均值分别为7.0×103cm~(-3)、7.5×103cm~(-3)、14.9×103cm~(-3)、1125μm2·cm~(-3)和50μm~3·cm~(-3)。香河地区积聚模态的粒子数浓度接近华北地区其他污染测站的结果,但高于发达国家的测值。冬季气溶胶的平均浓度最高(18.1×10~3cm~(-3)),而春季最低(12.3×10~3cm~(-3))。不同季节,气溶胶的数谱分布主要为单峰分布,平均峰值直径约为105 nm。气溶胶浓度的日变化受机动车排放的影响显著,存在早晚两个高值中心,分别出现在早上的06:00—09:00和晚上的19:00—21:00。风速、风向对气溶胶数浓度的影响较大,低风速(2 m/s)和南风条件,尤其是吹西南风时,气溶胶浓度的增加显著。     

南京北郊气溶胶中多环芳烃的污染特征及来源解析

利用2010年8月采集的南京北郊气溶胶样品,使用GC-MS对美国环保总局推荐的16种优先控制的多环芳烃含量、分布特征进行了研究。在此基础上,用特征比值法、主因子分析法分析得到南京市北郊大气中PAHs的主要来源为车辆尾气、燃煤、天然气和草木秸秆燃烧,并应用绝对因子分析法进一步定量计算主要源对PAHs的浓度贡献率。结果表明:1)大气颗粒物中16种多环芳烃的平均总质量浓度为135.85 ng/m~3,多环芳烃以4环为主,在可吸入颗粒物中的浓度占总浓度的88.7%;2)PM10中多环芳烃呈双模态分布,在9~10μm的粗模态和0.65~1.10μm的积聚模态上各出现一个峰值;3)天然气等对PAHs的贡献率为5.7%~44.1%,燃煤源的贡献率为20.7%~57.8%,汽车尾气的贡献率为4.6%~46.7%,木材燃烧的贡献率为2.9%~38.1%。本地交通排放和燃料燃烧是南京北郊大气颗粒物中PAHs的主要来源,远距离输送也对南京北郊气溶胶中的PAHs有重要贡献。     

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。     

New aerosol particle formation via certain ion driven processes

Ions can speed up the formation of aerosol particles. The former studies have mainly concerned on the role of the ion charge itself. We have studied the possible (additional) role of the actual small air ion spectrum shape, and the quantitative role of ion–ion recombination pathway. By means of our ion evolution model, formation of new species (H₂SO₄)_n(NH₃)_m(HNO₃)_k via ion–ion recombination was investigated. The model shows how the generation rate of the new species depends on the concentrations of H₂SO₄ and NH₃, and how it depends on the tropospheric background aerosol situation. The rate can be up to a few new neutral complexes per cubic centimeter and per second. New particle generation via ion–ion recombination provides an extra channel, especially for the clean atmosphere. Former results have shown that such situations are often present in Antarctica. Our aerosol spectrum measurements reveal a number of similar non-Antarctic results. Sometimes, such situations are followed by aerosol bursts, which may be (partly) due to an ion–ion recombination channel.     

Surface Tension Effects of Humic-Like Substances in the Aqueous Extract of Tropospheric Fine Aerosol

Organic aerosol constituents can influence the surface tension of nucleating cloud droplets and thereby modify the critical supersaturation necessary to activate aerosol particles. Model calculations, based on experiments carried out with different surrogates, led to contradictory conclusions on the effect of organic components on activation, indicating that the results depend very much on the surrogate selected. In order to reduce this uncertainty surface tension measurements were performed on real atmospheric aerosol components. Humic-like substances (HULIS) that accounted for 60% of the water-soluble organic carbon present in rural aerosol were isolated from 32 samples covering different seasons. The isolated organic matter present in a concentration of about 1 g L^–1, decreased the surface tension of the aqueous solutions by 25–42% as compared to pure water. This effect was further enhanced when humic-like substances were mixed with ammonium sulphate. In order to support model calculations Szyskowski functions were fitted to the data to formulate the surface tension effect as a function of concentration.Finally, natural humic substances (fulvic and humic acids) were investigated under the same conditions. The experiments revealed that the surface tension decreasing effect of atmospheric humic-like substances differed from that of the studied terrestrial and aquatic humic substances: the latter substances decreased the surface tension of the aqueous solution to a lesser extent (7–23%) than atmospheric HULIS. This deviation can be explained with the different composition (e.g. the ratio of aromatic to aliphatic moieties) of the substances investigated.     

Chemical Composition of Summertime PM2.5 and Its Relationship to Aerosol Optical Properties in Guangzhou, China

Urban aerosols have a large effect on the deterioration of air quality and the degradation of atmospheric visibility.Characterization of the chemical composition of PM 2.5 and in situ measurements of the optical properties of aerosols were conducted in July 2008 at an urban site in Guangzhou,Southern China.The mean PM 2.5 concentration for the entire period was 53.7±23.2 μg m 3.The mean PM 2.5 concentration (82.7±25.4 μg m 3) on hazy days was roughly two times higher than that on clear days (38.8±8.7 μg m 3).The total water-soluble ion species and the total average carbon accounted for 47.9%±4.3% and 35.2%±4.5%,respectively,of the major components of PM 2.5.The increase of secondary and carbonaceous aerosols,in particular ammonium sulfate,played an important role in the formation of haze pollution.The mean absorption and scattering coefficients and the single scattering albedo over the whole period were 53±20 M m 1,226±111 M m 1,and 0.80±0.04,respectively.PM 2.5 had a high linear correlation with the aerosol extinction coefficient,elemental carbon (EC) was correlated with aerosol absorption,and organic carbon (OC) and SO 4 2 were tightly linked to aerosol scattering.     

Size-Resolved Aerosol Characterization for a Polluted Episode at the IfT Research Station Melpitz in Autumn 1997

Inorganic ions, organic carbon (OC), elemental carbon (EC) and a variety of organic single species in airborne particles have been determined at the research station of the Leibniz – Institut für Troposphärenforschung (IfT) in Melpitz (Germany) in autumn 1997.Samples of eight selected measurement events were divided in two groups in order to investigate differences in the chemical composition of particles originating from southwesterly (SW – developed EU countries) or from easterly directions (E – less developed eastern countries). Differences between these two groups were tested statistically by Student's t-test.Five stage cascade impactor samples show nitrate as most abundant in the accumulation mode in the SW group. EC and sulphate show the most abundant mass fractions in the E group. That can be considered as a consequence of domestic coal heating and coal-fired power plant emissions in the region of westerly Poland, northern Czech Republic and easterly Germany. Higher nitrate concentrations in the SW group can be explained by stronger NO _x emissions caused by the leeward plume of the conurbation of Leipzig, as well as by the still higher traffic density in western Germany.The methane sulphonic acid (MSA) mass fraction was higher for SW air masses in accumulation mode particles, probably indicating marine origin. Succinic acid also showed higher mass fractions for the SW group. This could be caused by primary emission in automobile exhaust gases and photochemical formation during transport from SW. Indeed, during SW sampling, solar radiation intensity was higher than during E sampling.The observed differences in the particle composition are an expression of the still existing technology gradient in Europe. Future campaigns could show the development to a joint economy with smaller differences in anthropogenic emissions.     

重庆冬季大气气溶胶的物理、化学特征

利用2001—2002年重庆冬季大气气溶胶粒子观测资料，分析了气溶胶粒子的数浓度、质量浓度、谱分布、化学元素组成及其与气象因子的关系。结果表明，重庆冬季大气气溶胶数浓度与我国其他大城市处于同一水平，大于0．3μm气溶胶粒子的平均数浓度为225．3个／cm^3（最大337．8个／cm^3）；冷空气入侵和降水是局地气溶胶的主要清除机制，雾的存在可以显著地改变气溶胶数浓度的一般日变化规律；PM10占TSP（Total Suspended Particles，总悬浮颗粒物）质量浓度的60％～80％；人为污染元素S、zn、As、Ph等在细粒子中富集较高。     

北方沙尘气溶胶光学厚度和粒子谱的反演

利用CE-318太阳光度计在内蒙古额济纳旗、东胜、锡林浩特三地观测的2002年6月喇3年5月间的太阳直接辐射数据，应用消光法反演大气气溶胶光学厚度[AOT（λ），Aerosol Optical Thickness]和粒子谱分布，并分析其变化特征。结果表明，该地区气溶胶光学厚度具有明显的时空变化：春季最大，冬季最小，AOT（λ=440nm）平均最大值为0．78，最小值为0．13。3个观测点中，额济纳旗的光学厚度最大，东胜最小。光学厚度的日变化主要有4种形式：1）早晨高傍晚低；2）早晨低傍晚高；3）早晚低中午高；4）变化平缓。这主要与沙尘天气的发生、大气层结稳定度和人类活动等因素有关。气溶胶粒子谱分布基本符合Junge谱，在粒径0．3μm、0．6μm和1．0μm处出现峰值。但是在不同天气条件下粒子谱有很大差异，在沙尘暴天气中，大粒子和巨粒子数有明显的增加，粒子数浓度要比晴天背景大气大了约一个量级。春季气溶胶粒子数浓度最大，夏秋季次之，冬季最小，但相差不超过一个量级。     

Observed changes in aerosol physical and optical properties before and after precipitation events

Precipitation scavenging of aerosol particles is an important removal process in the atmosphere that can change aerosol physical and optical properties. This paper analyzes the changes in aerosol physical and optical properties before and after four rain events using in situ observations of mass concentration, number concentration, particle size distribution, scattering and absorption coefficients of aerosols in June and July 2013 at the Xianghe comprehensive atmospheric observation station in China. The results show the effect of rain scavenging is related to the rain intensity and duration, the wind speed and direction. During the rain events, the temporal variation of aerosol number concentration was consistent with the variation in mass concentration, but their size-resolved scavenging ratios were different. After the rain events, the increase in aerosol mass concentration began with an increase in particles with diameter 0.8 μm [measured using an aerodynamic particle sizer(APS)], and fine particles with diameter 0.1 μm [measured using a scanning mobility particle sizer(SMPS)]. Rainfall was most efficient at removing particles with diameter ～0.6 μm and greater than 3.5 μm. The changes in peak values of the particle number distribution(measured using the SMPS) before and after the rain events reflect the strong scavenging effect on particles within the 100–120 nm size range. The variation patterns of aerosol scattering and absorption coefficients before and after the rain events were similar, but their scavenging ratios differed, which may have been related to the aerosol particle size distribution and chemical composition.     

番禺秋季气溶胶浓度的变化与气象条件的关系

利用2004年9～11月在番禺区气象局采集到的气溶胶质量浓度资料和同期的气象资料,分析了番禺秋季气溶胶质量浓度变化及其与气象条件的关系。结果发现：番禺秋季大气污染物主要是PM10,PM10中以细粒子（PM2.5）为主,而且污染严重;气溶胶污染严重时大气层结稳定,污染高值主要出现在西北气流和东北气流的共同影响下,受周边环境的影响明显;PM（PM10和PM2.5）浓度超标日的天气过程主要出现在台风外围环流云系的影响下;气溶胶对能见度的影响较大,二者负相关明显。     

复合体系有机气体氧化生成二次有机气溶胶研究进展

生物源与人为源有机气体氧化形成的二次有机气溶胶(SOA)对气候变化和人类健康具有重要影响。SOA的产生与其前体物研究已取得了一些进展,但由于有机气体之间存在复合相互作用以及SOA形成机制复杂,目前对不同有机气体混合体系中SOA的形成认知还比较匮乏。因此,深入了解有机气体多源、复杂的相互作用,摸清有机气体的大气氧化机制、SOA的形成及影响等对深入理解真实大气有机气体化学演变具有指导意义。本文旨在了解复合体系有机气体氧化生成SOA的相关研究进展。一方面总结了复合体系有机气体产生SOA质量浓度、产率、成分、挥发性、光学性质等的变化,侧重于实验室复合体系有机气体氧化对SOA形成的多重影响以及SOA组成元素、分子构成的变化特征,并总结了目前实验室基于模型对复合体系SOA生成的模拟研究和拟合情况;另一方面探究了环境因素,如相对湿度(RH)、温度(T)以及无机气体,如氮氧化物(NO_x)、二氧化硫(SO₂)、氨气(NH₃)等对复合体系有机气体形成SOA的影响。     

兰州市区2002年春季3～4月近地层大气气溶胶的监测与分析

对兰州市区2002年春季3~4月近地层TSP连续观测资料进行分析,结果表明:(1)兰州市区TSP的质量浓度随着沙尘天气的发生而显著增加,沙尘天气越强,TSP的质量浓度越高,对兰州市区的空气污染越严重;(2)在不同天气情况下,兰州市区TSP与PM10的质量浓度有很好的对应关系,沙尘天气越强,其质量浓度都越高,但两者增减的比例各不相同;(3)在不同天气情况下,同级粒径粒子的质量浓度各不相同,但在同种天气情况下,各级粒径粒子质量浓度的分布规律却相同;(4)TSP样品色度的3个独立分量与空气质量有一定的对应关系,L*、a*、b*值越大,空气中沙尘含量越高,空气污染越严重,兰州市区在一般天气情况下L*、a*、b*值均较小,说明兰州市区空气污染主要以本地排放的黑色有机物为主。     

临安大气气溶胶理化特性季节变化

分别利用碳成分分析仪、离子色谱仪和原子吸收光谱仪等获取浙江省临安地区大气气溶胶在春、夏、秋、冬四季的质量浓度、离子与碳成分特性,并对不同粒径气溶胶成分分布特点作了较详细分析。结果表明：气溶胶质量浓度、可溶性离子浓度以及碳成分浓度具有明显的季节变化趋势。整个尺度范围内,气溶胶质量浓度季节变化特点为春季浓度最高,达到534 μg/m3;冬季次之,质量浓度为117.21 μg/m3;夏季浓度最低,平均为65.7 μg/m3;秋季质量浓度98.6 μg/m3。可溶性离子成分在气溶胶中所占比例具有明显的季节性,其中夏季最高为49.4%,春季最低为11.3%。硫酸根离子SO42-和氨根离子NH4+和硝酸根离子NO3- 3种离子浓度之和约占离子总量的75%~83%。受温度影响,硝酸根离子NO3-浓度随季节变化幅度较大,夏季平均浓度为1.7 μg/m3, 冬季平均浓度为11.5 μg/m3,是夏季浓度的6.8倍。碳浓度分布特点显示,气溶胶中元素碳浓度春季最高,夏季最低。有机碳浓度春季最高,冬季最低。气溶胶粒度分布特点也非常明显。四季中粒径小于11 μm（PM11）的气溶胶均占气溶胶总量的90%以上,粒径小于2.1 μm（PM2.1）的气溶胶占到气溶胶总量的53%以上。可溶性离子在粒径小于2.1 μm气溶胶颗粒中,以硫酸根离子、氨根离子和硝酸根离子为主。碳成分尺度分布特征为颗粒越小,有机碳及元素碳浓度越高。