2006年北京春季气溶胶吸收系数的分离研究

对2006年春季北京城区大气气溶胶中沙尘和黑碳气溶胶吸收系数的波长指数及其对总吸收系数的贡献进行了估算。结果表明：2006年春季北京城市地区测点,黑碳气溶胶吸收系数随波长的变化呈指数递减,假设某些天的气溶胶吸收无沙尘的贡献,估算的波长幂指数a＝-0.92。另外,计算了北京3次浮尘天气下沙尘气溶胶对吸收系数（520 nm波段）的贡献,计算表明,在浮尘天气影响期间,沙尘气溶胶对吸收系数的贡献平均为32.8%,黑碳气溶胶仍是浮尘影响期间城市气溶胶吸收消光的主要物质。     

有关气溶胶细粒子对城市能见度影响的研究

文章介绍了国外关于大气气溶胶细粒子对城市能见度影响的研究情况。城市能见度降低问题是由气溶胶PM10、PM2.5和NO2气体引起的。影响城市能见度的颗粒物的主要来源是：机动车尾气（29％）、煤灰（18％）、二次硫酸盐（17％）、生物质燃烧（10％），自然源、海盐、土壤/公路边灰尘各贡献（2％）。     

雾天气向霾天气转化时气溶胶颗粒物的动力学特性

针对自然界中雾天气向霾天气转化的现象,提出建立和发展雾环境气溶胶颗粒物多效应的动力学模型。基于离散系统的颗粒群平衡方程和多重Monte Carlo算法,分别对雾形成阶段（凝并、冷凝和成核3个动力学事件占主导）、雾发展阶段（凝并、破碎、沉积和成核4个动力学事件占主导）和雾消散阶段（破碎、蒸发和沉积3个动力学事件占主导）气溶胶颗粒物平均体积、颗粒数目随时间的演变过程进行研究。结果表明：气溶胶颗粒物的初始体积尺度为1,经过雾的生命周期进入消散阶段时,尺度为0.0156的细小气溶胶颗粒数目迅速增加,1000 s时间已发展至初始值的8.12倍。研究结果解释了自然界中雾天气向霾天气转化的过程和物理机制。     

无人直升机搭载大气颗粒物采样装置的前期地面评估

与搭载气溶胶观测和分析仪器测量相比,利用无人直升机搭载气囊采集高空大气颗粒物是一种经济、便捷和安全的采集方式。为了解无人直升机采样装置的采样效果,选择2014年10月至2015年3月的4次重污染天气过程,由无人直升机搭载气囊采集大气颗粒物,然后利用气溶胶采样器采集气囊内的大气颗粒物样品并计算采样时间,再利用气溶胶采样器采集相同时间段内的地面大气颗粒物(气囊外),并将两者进行对比。结果表明:在稳定的污染天气条件下,采集气囊内的大气颗粒物,与相同时间段内利用气溶胶采样器直接采集气囊外的大气颗粒物相比,两种方式采集到的大气颗粒物质量最大差值29%,最小差值11%,平均为21%;利用无人直升机的大气采样装置采集大气颗粒物对碳气溶胶组分影响很小,气囊内与气囊外OC/TC最大相差2.0%,最小相差0.5%。上述结果表明,无人直升机的大气采样装置有比较好的采集效率,利用气囊这种经济、便捷、安全的方式,搭载在无人机平台上,采集高空大气是一种获取气溶胶垂直廓线的有效方法,有望在未来的气溶胶气候和环境研究中提供宝贵数据。     

北京春季沙尘和霾期间气溶胶的对比模拟研究

利用气象模式WRF驱动区域空气质量模式RAQMS,模拟研究了2014年北京地区春季颗粒物及气溶胶化学组分的时空变化,对比分析了沙尘期（3月17日、29日）和霾期（3月25～27日）的天气形势、气象要素和气溶胶化学组分特征,比较了沙尘和人为气溶胶表面非均相化学反应对大气化学成分的影响及相对贡献。结果显示,模式对于气象要素、PM2.5、PM10及其化学组分具有较好的模拟能力,考虑了气溶胶表面非均相化学反应后明显提高了模式对PM2.5及气溶胶化学组分模拟的准确性。沙尘期间,沙尘对PM10质量浓度贡献占主导地位（50.7%）,对PM2.5的贡献与有机气溶胶（OM）和人为排放的一次颗粒物（PPM）相当;霾期间,硝酸盐NO₃?（25.6%）和OM（23.6%）对PM2.5的贡献最大,在PM10中NO₃?、PPM和OM的贡献相当。沙尘期,粗粒子明显增加,在PM10中所占比例与细粒子相当,为45.5%;霾期,细粒子占主导地位,占PM10质量浓度的85.6%。非均相化学反应使沙尘期间硫酸盐（SO₄2–）和NO₃–浓度分别增加16.9%和83.8%,使霾期间的SO₄2?和NO₃–浓度分别增加14.5%和45.0%。2014年3月,非均相化学反应使北京月均SO₂、NO₂、O₃、SO₄2?、NH₄+和NO₃?的浓度分别变化了?2.5%、?5.7%、?3.4%、11.7%、18.6%和58.5%,本文结果表明非均相化学反应对二次无机气溶胶的生成有重要贡献。     

北京上甸子典型天气个例的大气气溶胶数谱分布特征

使用差分淌度粒径分析仪(TDMPS)和空气动力学粒径分析仪(APS)对上甸子区域本底站气溶胶(直径3nm~10μm)数谱分布特征进行观测。利用2008年的观测结果,分析了不同天气(包括沙尘天气、干洁天气和雾霾天气)条件下大气气溶胶数谱分布及其与气象要素和气团来源的关系。结果表明,沙尘天气条件下,上甸子站受西北方向的气团控制,风速较大,粗粒子数浓度明显增加,PM10的质量浓度可以迅速增加到毫克每立方米(mg·m-3)的量级。典型的"香蕉型"新粒子生成事件通常发生在比较干洁晴朗的天气条件下,西北气团主导,大气中背景气溶胶数浓度较低,核模态气溶胶数浓度迅速增长,气溶胶的粒径呈现明显的增长过程,核模态可以平稳地增长到约80nm,达到成为云凝结核的尺度。雾霾天气通常是在西南气团影响下,细颗粒物(1μm以下)不断累积、相对湿度不断升高的条件下发生的。雾霾天气条件下数谱分布的几何中值粒径出现在积聚模态,积聚模态数浓度也高于非雾霾天。个例研究表明,雾霾天气条件下,PM2.5质量浓度可以达到非雾霾天的10倍左右,其中以细颗粒物的贡献为主。在雾霾天气条件下,上甸子站数浓度较高的积聚模态颗粒物主要来自城区的传输,因此对背景地区气溶胶数谱的研究可以为解析城区气溶胶复杂来源提供依据。     

武汉市科教区冬春季气溶胶的元素组成特征及来源分析

2006-2007年冬春季在武汉市湖北大学校区连续采集气溶胶样品,测定气溶胶元素组成,分析气溶胶样品总悬浮颗粒物（TSP）质量浓度,再结合污染源的特征元素组成来确定污染物的来源构成。结果表明：湖北大学校区大气气溶胶污染程度较轻,气溶胶元素以地壳元素为主,其次是具有代表性的人为污染物元素,再次是盐类元素。通过因子载荷分析和相关性分析显示,湖北大学周边地区的建筑源、交通源和餐饮源是湖北大学校区大气的主要污染源。     

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。     

南京市主城区大气颗粒物来源探讨

在2005-05-03——05-27期间,用Anderson九级采样器在南京市两个采样点采集大气气溶胶样品,同时进行了部分排放源的采集。用X射线—荧光光谱仪(XRF)分析得到气样及源样中PM10的化学成分,分析了南京市大气气溶胶的元素质量谱分布,进行了PM10的富集因子分析,并应用化学质量平衡法(CMB)计算各类源对气溶胶PM10的贡献。结果表明,各类污染源对南京市气溶胶PM10的贡献率分别为:建筑尘(35.45%)、煤烟尘(22.13%)、土壤尘(20.27%)、硫酸盐(5.43%)、汽车尘(4.61%)、海盐(1.91%)、冶炼尘(1.69%)、其它源(8.51%)。文中还结合了南京市TSP和PM2.5的来源解析结果,分析了南京市不同粒径气溶胶颗粒物的污染特征。     

南京市总悬浮颗粒物（TSP）及地面积尘来源解析

本文使用受体模型中的化学元素平衡法（CMB）对南京市的大气总量浮颗粒物（TSP）来源进行解析研究，同时对地面积尘进行解析，结果表明建筑尘对TSP的贡献为31％－45％，位列第一，其次是煤烟（20％－38％），土壤尘（15％－23％），冶炼尘（＜3％），对地面积尘的解析结果也与TSP相同，该文的结果为污染物的防治提供决策依据。     

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。     

Transformation of Aerosol Chemical Properties due to Transport Over a City

The change of the chemical composition of the near-ground level atmospheric aerosol was studied during two summer episodes by a Lagrangian type of experimental approach. Bulk and single-particle chemical analyses of ions and elements in the particulate phase were deployed. N(-III) and N(V) components were also measured in the gas-phase. The measurements were completed by particle size distributions.Secondary inorganic aerosols (SIA) and fine particles of ≈0.2–0.4 μm size were still elevated 50 km downwind of the city. The direct comparison of transport over the city in contrast to transport over the surrounding areas showed that SIA was formed from emission from the city within less than 3 h. Relative increases, i.e., enrichment during transport were observed for primary and secondary aerosol components. The degree of mixing on the individual particle level increased significantly during transport in the area. In particular, newly emitted carbonaceous particles became internally mixed within hours with pre-existing sulphate particles. Mostly due to secondary aerosol formation the average particle size (mass median diameter) of major constituents of the aerosol was significantly decreased while being transported over 13 h. Given recent insights which link fine particles number and mass concentrations with health risks, the results suggest that rural populations in areas which frequently are located within an urban plume might run an elevated health risk relative to populations in areas not affected by urban plumes.     

SEM-EDX Characterisation of Tropospheric Aerosols in the Negev Desert (Israel)

Individual aerosol particles collected in the Negev desert in Israel during a summer and winter campaign in 1996–1997 were analysed by scanning electron microscopy with energy-dispersive X-ray analysis. Hierarchical cluster analysis was performed to interpret the data on the basis of particle diameter and composition. Eleven particle classes (groups) provided clues on sources and/or particle formation. The summer samples were enriched in sulphates and mineral dusts; the winter samples contained more sea salts, aged sea salts, and industrial particles. The fine size fraction below 1 m diameter was enriched in secondary particles and showed evidence of atmospheric processing. The secondary sulphate particles were mainly attributed to long-range transport. A regional conversion from calcite to calcium sulphate occurred during summer. Industrial particles originating from local pollution appeared during winter.     

Growth Rates of Fine Aerosol Particles at a Site near Beijing in June 2013

Growth of fine aerosol particles is investigated during the Aerosol–CCN–Cloud Closure Experiment campaign in June2013 at an urban site near Beijing. Analyses show a high frequency(~ 50%) of fine aerosol particle growth events, and show that the growth rates range from 2.1 to 6.5 nm h~(-1) with a mean value of ~ 5.1 nm h~(-1). A review of previous studies indicates that at least four mechanisms can affect the growth of fine aerosol particles: vapor condensation, intramodal coagulation,extramodal coagulation, and multi-phase chemical reaction. At the initial stage of fine aerosol particle growth, condensational growth usually plays a major role and coagulation efficiency generally increases with particle sizes. An overview of previous studies shows higher growth rates over megacity, urban and boreal forest regions than over rural and oceanic regions. This is most likely due to the higher condensational vapor, which can cause strong condensational growth of fine aerosol particles.Associated with these multiple factors of influence, there are large uncertainties for the aerosol particle growth rates, even at the same location.     

Using Föhn conditions to characterize urban and regional sources of particles

Characterizations of urban and regional sources of particulate matter (PM) were performed in the Milan area (North of Italy) during Föhn and stagnant (non-Föhn) conditions. The measurements were performed at two different places: in an urban area North of Milan (Bresso) and in a regional area at the EMEP-GAW station in Ispra (about 65 km NW from Milan) during the winter periods of the years 2002–2007. Particle size distributions and chemical bulk analysis of aerosols are combined with single particle mass spectrometry to obtain information about the chemical content of the particles and their mixing state. Föhn conditions are characterized by extremely clean background air from which background aerosol is scavenged, and consequently local sources (here defined as sources between the sampling sites and the mountain range top about 100–150 km away depending on the wind direction) determine the aerosol properties.It was observed that during Föhn events the accumulation mode in the size range 50 nm < d < 300 nm practically disappears and that the size fraction below 50 nm dominates the total number distribution. The significant change in the number size distribution and the large decrease in PM10 mass during Föhn events are accompanied by a significant change in the chemical composition of the particles. Results from bulk chemical analysis showed high amounts of carbonaceous compounds and very low concentrations of ammonium nitrate (as indicator for secondary chemistry) during Föhn episodes, in contrast to stagnant conditions, when secondary components are dominating the aerosol composition. Single particle measurements confirm the high contribution of carbonaceous compounds in locally emitted particles.It was concluded that particles that originated in the urban area come mainly from combustion processes, especially direct traffic emissions, domestic heating and industrial activities, whereas the regionally emitted particles are different with much less traffic contribution.We estimate that under prevailing (non-Föhn) winter conditions, about 50–65% of the aerosol mass load in the city of Milan are caused by local emissions, and about 35–50% come from regional background. This finding suggests that in order to improve air quality in a big city like Milan, it is important to combine local traffic restriction interventions with other long-term regional scale air-quality-measures.     

Carbonaceous materials in size-segregated atmospheric aerosols from urban and coastal-rural areas at the Western European Coast

A high-volume cascade impactor, equipped with a PM10 inlet, was used to collect size-segregated aerosol samples during the summer of 2004 at two Portuguese locations: a coastal-rural area (Moitinhos) and an urban area (Oporto). Concentrations of airborne particulate matter (PM), total carbon (TC), organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC) were determined for the following particle size ranges: < 0.49, 0.49–0.95, 0.95–3.0, and 3.0–10 µm. The total PM mass concentrations at the urban and coastal-rural sites ranged from 22.8 to 79.6 μg m^− 3 and 19.9 to 28.2 μg m^− 3, respectively, and more than 56% of the total aerosol mass was found in the fractions below 3.0 μm. At both locations the highest concentrations of OC and EC were found in the submicrometer size range. The regional variability for the OC and EC concentrations, with the highest concentrations being found in the urban area, was related to the contribution of local primary sources (mostly traffic emissions). It was also verified an enrichment of the small size particles in WSOC, representing on average 37.3(± 12.4)% and 59.7(± 18.0)% of OC in the very fine aerosol at the coastal-rural and urban areas, respectively. The amount of secondary OC calculated by the minimum OC/EC ratio method indicates that secondary organic aerosol formation was important throughout the study at both sites. The obtained results suggest that long-range transport and favourable summer conditions for photochemical oxidation are key factors determining secondary OC formation in the coastal-rural and urban areas. The ultraviolet absorption properties of the chromophoric constituents of the WSOC fractions were also different among the different particle size ranges and also between the two sampling locations, thus suggesting the strong impact of the diverse emission sources into the composition of the size-segregated organic aerosol.     

Carbonaceous materials in size-segregated atmospheric aerosols from urban and coastal-rural areas at the Western European Coast

A high-volume cascade impactor, equipped with a PM10 inlet, was used to collect size-segregated aerosol samples during the summer of 2004 at two Portuguese locations: a coastal-rural area (Moitinhos) and an urban area (Oporto). Concentrations of airborne particulate matter (PM), total carbon (TC), organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC) were determined for the following particle size ranges: < 0.49, 0.49–0.95, 0.95–3.0, and 3.0–10 µm. The total PM mass concentrations at the urban and coastal-rural sites ranged from 22.8 to 79.6 μg m^− 3 and 19.9 to 28.2 μg m^− 3, respectively, and more than 56% of the total aerosol mass was found in the fractions below 3.0 μm. At both locations the highest concentrations of OC and EC were found in the submicrometer size range. The regional variability for the OC and EC concentrations, with the highest concentrations being found in the urban area, was related to the contribution of local primary sources (mostly traffic emissions). It was also verified an enrichment of the small size particles in WSOC, representing on average 37.3(± 12.4)% and 59.7(± 18.0)% of OC in the very fine aerosol at the coastal-rural and urban areas, respectively. The amount of secondary OC calculated by the minimum OC/EC ratio method indicates that secondary organic aerosol formation was important throughout the study at both sites. The obtained results suggest that long-range transport and favourable summer conditions for photochemical oxidation are key factors determining secondary OC formation in the coastal-rural and urban areas. The ultraviolet absorption properties of the chromophoric constituents of the WSOC fractions were also different among the different particle size ranges and also between the two sampling locations, thus suggesting the strong impact of the diverse emission sources into the composition of the size-segregated organic aerosol.     

Using Föhn conditions to characterize urban and regional sources of particles

Characterizations of urban and regional sources of particulate matter (PM) were performed in the Milan area (North of Italy) during Föhn and stagnant (non-Föhn) conditions. The measurements were performed at two different places: in an urban area North of Milan (Bresso) and in a regional area at the EMEP-GAW station in Ispra (about 65 km NW from Milan) during the winter periods of the years 2002–2007. Particle size distributions and chemical bulk analysis of aerosols are combined with single particle mass spectrometry to obtain information about the chemical content of the particles and their mixing state. Föhn conditions are characterized by extremely clean background air from which background aerosol is scavenged, and consequently local sources (here defined as sources between the sampling sites and the mountain range top about 100–150 km away depending on the wind direction) determine the aerosol properties.It was observed that during Föhn events the accumulation mode in the size range 50 nm < d < 300 nm practically disappears and that the size fraction below 50 nm dominates the total number distribution. The significant change in the number size distribution and the large decrease in PM10 mass during Föhn events are accompanied by a significant change in the chemical composition of the particles. Results from bulk chemical analysis showed high amounts of carbonaceous compounds and very low concentrations of ammonium nitrate (as indicator for secondary chemistry) during Föhn episodes, in contrast to stagnant conditions, when secondary components are dominating the aerosol composition. Single particle measurements confirm the high contribution of carbonaceous compounds in locally emitted particles.It was concluded that particles that originated in the urban area come mainly from combustion processes, especially direct traffic emissions, domestic heating and industrial activities, whereas the regionally emitted particles are different with much less traffic contribution.We estimate that under prevailing (non-Föhn) winter conditions, about 50–65% of the aerosol mass load in the city of Milan are caused by local emissions, and about 35–50% come from regional background. This finding suggests that in order to improve air quality in a big city like Milan, it is important to combine local traffic restriction interventions with other long-term regional scale air-quality-measures.     

Single Particle Characterisation of the Aerosol in the Marine Boundary Layer and Free Troposphere over Tenerife, NE Atlantic, during ACE-2

In the framework of the 2nd Aerosol Characterization Experiment (ACE-2), in June and July 1997, size segregated samples were collected for single particle analysis on the island of Tenerife, in both the marine boundary layer (MBL) and the free troposphere (FT), to study the characteristics of the North Atlantic aerosol. A systematic assessment was made of the aerosol under background conditions and when the environment was perturbed by European emissions and/or Saharan dust. The aerosol particles were analysed by automated and manual SEM-EDX, followed by cluster analysis to identify the different particle types and their abundance. Basing on back trajectory calculations, particle numbers and volume concentrations, different periods can be identified regarding the origin of the sampled air masses. In the FT, the air masses were classified as clean Atlantic, Saharan dust from Africa or pollution from Europe. In the MBL, air masses were classified as clean, polluted or perturbed by emissions from Europe. For both the FT and MBL samples, the main changes in chemical composition were observed between the fine and coarse mode aerosol. The FT fine mode aerosol is dominated by S-poor aluminosilicates (62%) in the event of the dust samples or sulphates, carbonaceous particles (20%) and S-rich aluminosilicates (46%) in the polluted samples. For the larger fractions, a strong decreasing trend was observed for the sulphates (less than 20%) and carbonaceous particles (10%) in the polluted samples. The MBL fine mode was completely dominated by S-rich particles (polluted 55% and perturbed 59%), and to a lesser extent, carbonaceous and aged sea salt particles. In the coarse mode, the polluted air mass is dominated by sea salt particles (62%). Contrary to the fine fraction, the polluted air mass in the coarse fraction contained 5.3% of S-rich particles. The combined interpretation of the data from the analysis of size-fractioned particles and the calculated backward trajectories for air masses coming from Europe, Africa and the Atlantic, results in better insights on aerosol chemistry, especially for the comparison of the particle composition in the FT and the MBL.     

2004年北京秋季大气颗粒物的化学组分和来源特征

2004年9月在北京城区进行了大气颗粒物采样,样品用PIXE方法进行了分析,得到了20种元素的浓度及其谱分布。并对北京颗粒物的谱分布、富集因子和来源进行了分析研究。发现K元素浓度分布呈细粒态单峰谱分布,细粒态K富集因子较高,表明了生物质燃烧的主要贡献。因子分析结果还表明,土壤尘、生物质燃烧、煤烟尘、工业源和汽车尾气排放源对秋季北京局地排放源有明显贡献。