大气气溶胶细粒子研究进展

大气细粒子PM2.5是大气气溶胶的一个组成部分,由于其粒径小,比表面积大,可以为有毒物质提供载体,所以它对环境和人体健康都有很大的影响。本文主要从PM2.5的危害、研究方法和沙尘细粒子的研究进展来阐述国内外细粒子的研究现状,并对其今后研究热点及新方向进行了展望。     

珠江三角洲大气灰霾导致能见度下降问题研究

大气气溶胶的气候效应和环境效应研究是当今国际科技界的热门话题。近年来珠江三角洲地区的气溶胶污染日趋严重,一年四季长期稳定存在气溶胶云,重污染区偏于珠江口以西的珠江三角洲西侧。灰霾天气主要出现在10月至次年4月。大气灰霾导致能见度恶化。自20世纪80年代初开始,该地区的能见度急剧恶化,灰霾天气显著增加,其中有3次大的波动,分别代表与珠江三角洲经济发展相伴随的气溶胶污染、硫酸盐加气溶胶污染、光化学过程的细粒子加硫酸盐加气溶胶的复合污染时期。雾和轻雾造成的低能见度的长期变化趋势,没有由于人类活动影响或经济发展影响带来的趋势性变化,其波动主要反映了气候波动固有的年际和年代际变化。珠江三角洲能见度的恶化主要与细粒子关系比较大,PM10有一半月均值超过国家二级标准的日均值浓度限值(150μg/m3),而PM2.5月均值全部超过美国国家标准的日均值浓度限值(65μg/m3),尤其是10月至次年1月的月均值浓度几乎超过标准限值的1倍,细粒子浓度甚高。另外PM2.5占PM10的比重非常高(58%—77%),尤其是旱季比雨季更高。与15a前的资料相比较,细粒子在气溶胶中的比重有明显增加,因而在目前珠江三角洲的气溶胶污染中,主要是细粒子的污染。     

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。     

北京市大气细粒子质量浓度与能见度定量关系初探

北京近年的监测结果表明,大气中通过消光作用使大气能见度下降的气溶胶细粒子的污染水平呈现上升趋势。中国气象局北京城市气象研究所与北京大学合作于2001年春季(3月)、夏季(6月)、秋季(9月)和冬季(12月)开展了大气细粒子与气象能见度的同步综合观测,旨在探求细粒子的物理化学特征及其与大气能见度的关系。监测结果表明,能见度与PM2.5质量浓度在春季呈乘幂关系;夏季除高相对湿度外,呈指数关系;秋季呈对数关系;冬季呈指数关系。为了便于比较,将两者间的关系全部用指数关系表示。北京市大气能见度与细粒子质量浓度呈现很好的负相关性,无疑细粒子污染是造成大气能见度下降的主要原因,它已成为目前中国大气污染研究的重要内容之一。     

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％）。     

2008年北京奥运会期间大气气溶胶物理特征分析

应用MODIS卫星的气溶胶产品资料和地面的光学粒子计数器的资料,对比分析了北京地区2006、2007、2008年7～9月的气溶胶光学厚度、细粒子光学厚度、Angstrom指数、气溶胶粒子数浓度谱及体积谱,发现2008年北京奥运会期间(7月20日～9月20日)的气溶胶光学厚度比2006、2007年同期明显降低,气溶胶细模态光学厚度占总光学厚度的比上升,Angstrom指数上升,气溶胶细粒子数浓度没有明显相对变化,而粗粒子数浓度则减少约50%.利用大气标高,将MODIS反演的气溶胶柱的质量浓度转化为地面气溶胶质量浓度.用粒子计数器得到的体积谱,在假定气溶胶粒子密度的情况下,计算出其质量浓度.将这两种方法得到的气溶胶质量浓度与国家环境保护部公布的空气质量指数换算得到的可吸入颗粒物(PM10)质量浓度进行比较.结果表明:北京奥运期间空气质量总体达到了国家二级空气质量标准;与2006、2007年同期相比,2008年气溶胶PM10质量浓度明显下降,而这主要是由气溶胶粗粒子的减少引起的.     

一次热带气旋外围下沉气流造成的珠三角地区连续灰霾天气过程分析

通过研究广州番禺大气成分站的气溶胶颗粒物质量浓度(PM10和PM2.5)、黑碳浓度、臭氧浓度等大气成分要素,常规地面气象要素以及气流后向轨迹、垂直速度、位温和边界层高度等资料,结合热带气旋路径和天气形势对热带气旋外围下沉气流造成的一次珠三角地区连续灰霾天气过程的形成原因和变化特征进行了分析.由于热带气旋移动缓慢,其外围下沉气流使珠三角地区形成了层结稳定、静小风和晴朗少云的天气条件,导致珠三角地区出现连续的灰霾天气.在这次灰霾过程中,气溶胶粒子来源以本地源为主,并且以细粒子为主,PM2.5占PM10的比例接近70％,黑碳浓度占PM10的6.0％左右;在凌晨,由于边界层高度降至最低,垂直扩散条件差,同时相对湿度也达到峰值,气溶胶吸湿增长明显,易出现能见度低值.     

太原冬季大气气溶胶的散射特征

利用积分浊度仪于2005年12月17日-2006年2月14日对太原市区气溶胶散射特性进行了观测分析。结果表明：观测期间气溶胶散射系数小时平均值为（850.2±611.3) Mm-1,散射系数在200～300 Mm-1之间出现的频率最高。太原冬季大气气溶胶散射系数的日变化呈双峰型,散射系数与PM2.5小时平均浓度的线性相关性较好（R2 = 0.82),表明细粒子对散射系数有很大的贡献。观测结果显示气象条件是影响气溶胶散射特性的重要因素之一。     

南海夏季风撤退期的气候特征I——40年平均

近年来广州地区的气溶胶污染日趋严重,灰霾天气主要出现在10月～次年4月。大气灰霾导致能见度恶化。自1980年代初开始,该地区的能见度急剧恶化,灰霾天气显著增加,其中有3次大的波动,分别代表广州地区经济发展相伴随的粉尘污染、硫酸盐加粉尘污染、光化学过程的细粒子加硫酸盐加粉尘的复合污染时期。雾和轻雾造成的低能见度的长期变化趋势,没有由于人类活动影响或经济发展影响带来的趋势性变化,其波动主要反映了气候波动固有的年际和年代际变化。广州地区能见度的恶化主要与细粒子有关,PM10有一半季均值超过国家二级标准的日均值浓度限值,而PM2.5季均值全部超过美国国家标准的日均值浓度限值,细粒子浓度甚高。另外PM2.5占PM10的比重非常高,可达62%～69%,尤其是旱季比雨季更高。     

2007年春季广州城区黑碳气溶胶污染特征的初步研究

2007年4月利用黑碳仪（Aethalometer）、颗粒物在线观测仪（TEOM1400a）和现时天气现象传感器（PWD22）获得了大气细粒子中每5 min黑碳气溶胶（BC）浓度以及每30 min PM2.5浓度及大气能见度观测数据。结果发现：黑碳日均值浓度为7.4±2.9 μg·m－3,变化范围分别为2.1～11.6 μg·m－3。PM2.5日均值浓度为77.4±35.9 μg·m－3,浓度变化范围分别为29.6～183.3 μg·m－3。黑碳小时浓度变化具有2个明显的峰值,主要与机动车尾气排放密切相关。黑碳浓度与PM2.5浓度呈正相关,与大气能见度呈负相关,相关系数为分别为0.707和－0.529,表明黑碳是PM2.5中的重要组成部分,对大气能见度的影响较显著。     

沙尘传输路径上气溶胶浓度与干沉降通量的粒径分布特征

利用2002年春季中国北京、青岛和日本福冈3个地区的分级气溶胶浓度资料,结合改进的Wil-liams模型,分析了沙尘传输路径上空气动力学直径≤11μm气溶胶(PM11)浓度和干沉降通量的粒径分布特征,并估算了黄海海域春季PM11的干沉降通量及不同粒径气溶胶的贡献。结果表明:3个地区PM11浓度粒径分布在非沙尘时期呈双峰分布,两个峰值分别出现在细颗粒(<2.1μm)部分和粗颗粒(2.1～11μm)部分;沙尘时期,3个地区PM11浓度粒径分布均趋于单峰分布,峰值位于粗颗粒部分,并且越靠近沙尘源地,这种趋势越明显。较强沙尘天气时期,粗颗粒部分的浓度峰值粒径从沙尘源地附近到黄海西岸、东岸呈降低趋势,但在一般沙尘天气时期,这种现象并不明显。沙尘时期和非沙尘时期,3个地区粗颗粒的干沉降通量均随粒径增加而增大,细颗粒的干沉降通量随粒径的变化不明显。虽然沙尘时期粗颗粒沉降通量较非沙尘时期有明显增加,但粗颗粒对PM11干沉降通量的贡献与非沙尘时期相比,并没有明显的变化。较强沙尘天气时期,3个地区粗颗粒的干沉降通量明显高于一般沙尘天气时期;细颗粒的干沉降通量较一般沙尘天气时期略有增加。黄海海域春季沙尘时期PM11的干沉降通量约为31.70～58.59mg.m-2.d-1,非沙尘时期约为8.33～15.94mg.m-2.d-1。粗颗粒是黄海海域春季PM11干沉降通量的主要贡献者,约占PM11干沉降通量的94.2%以上。     

Chemical composition of PM2.5 at an urban site of Chengdu in southwestern China

PM2.5 aerosols were sampled in urban Chengdu from April 2009 to January 2010, and their chemical compositions were characterized in detail for elements, water soluble inorganic ions, and carbonaceous matter. The annual average of PM2.5 was 165g m－3, which is generally higher than measurements in other Chinese cities, suggesting serious particulate pollution issues in the city. Water soluble ions contributed 43.5% to the annual total PM2.5 mass, carbonaceous aerosols including elemental carbon and organic carbon contributed 32.0%, and trace elements contributed 13.8%. Distinct daily and seasonal variations were observed in the mass concentrations of PM2.5 and its components, reflecting the seasonal variations of different anthropogenic and natural sources. Weakly acidic to neutral particles were found for PM2.5. Major sources of PM2.5 identified from source apportionment analysis included coal combustion, traffic exhaust, biomass burning, soil dust, and construction dust emissions. The low nitrate: sulfate ratio suggested that stationary emissions were more important than vehicle emissions. The reconstructed masses of ammonium sulfate, ammonium nitrate, particulate carbonaceous matter, and fine soil accounted for 79% of the total measured PM2.5 mass; they also accounted for 92% of the total measured particle scattering.     

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。     

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.     

Spatio-temporal variations of optical properties of aerosols in East Asia measured by MODIS and relation to the ground-based mass concentrations observed in central Korea during 2001∼2010

Long-term variations and trends of atmospheric aerosols in the East Asian region were analyzed by using aerosol optical depth (AOD or τ), and ångström exponent (AE or α) obtained from the Moderate Resolution Imaging Spectroradiometer (MODIS) from 2001 to 2010. The increased emission of anthropogenic fine aerosols in east China resulted in the high AOD in this region during summer. The steady increasing emission of anthropogenic fine aerosols caused an increasing trend of AOD in east China, and the large-scale transport of sandstorms and smoke plume caused by forest fires affected intense inter-annual variations of AOD in the East Asian region. While in the central part of South Korea, located in the lee side of the East Asian continent, AE tended to rise to a level higher than in east China, the ground-based mass concentrations continued to decline. A noticeable decrease of PM10 mass concentration in spring and winter in central Korea is most likely attributable to decreases in sandstorms in the source region of East Asia. However, the ratio of PM2.5 mass concentration to PM10 increases overall with a high level in summer. Aerosol types were classified into dust, smoke plume, and sulphate by using satellite data over Cheongwon in central Korea. The columnar AOD, with different aerosol types, was compared with the ground-based mass concentrations at Cheongwon, and the relatively high level of the correlations presented between PM2.5 and AOD produced in sulphate. Growth and increases of fine hygroscopic aerosols generated as gas-to-particle conversion particularly in summer contribute to increases of columnar AOD in the East Asian region.     

Characteristics of Chemical Speciation in PM_1 in Six Representative Regions in China

A better knowledge of aerosol properties is of great significance for elucidating the complex mechanisms behind frequently occurring haze pollution events. In this study, we examine the temporal and spatial variations in both PM_1 and its major chemical constituents using three-year field measurements that were collected in six representative regions in China between 2012 and 2014. Our results show that both PM_1 and its chemical compositions varied significantly in space and time, with high PM_1 loadings mainly observed in the winter. By comparing chemical constituents between clean and polluted episodes, we find that the elevated PM_1 mass concentration during pollution events should be largely attributable to significant increases in organic matter(OM) and inorganic aerosols like sulfate, nitrate, and ammonium(SNA),indicative of the critical role of primary emissions and secondary aerosols in elevating PM_1 pollution levels. The ratios of PM_1/PM_(2.5) are found to be generally high in Shanghai and Guangzhou, while relatively low ratios are seen in Xi'an and Chengdu, indicating anthropogenic emissions were more likely to accumulate in forms of finer particles. With respect to the relative importance of chemical components and meteorological factors quantified via statistical modeling practices, we find that primary emissions and secondary aerosols were the two leading factors contributing to PM_1 variations, though meteorological factors also played important roles in regulating the dispersion of atmospheric PM.     

2010-2011年鞍山市能见度特征

利用2010年6月至2011年5月鞍山大气成分观测站的能见度资料,统计分析能见度与PM₁₀、PM_2.5、PM_1.0质量浓度、风速、降水强度和气溶胶光学厚度等气象要素的相关性。结果表明：鞍山市能见度月均值从8月份开始呈上升趋势,11月份达到峰值后开始显著下降,2月份达到最低值,自3月开始又出现较大幅度增长,进入夏季后略有下降;PM_2.5/PM₁₀、PM_1.0/PM₁₀比值与能见度呈反相关,能见度增大,PM_2.5/PM₁₀、PM_1.0/PM₁₀比值减小,且PM_1.0/PM₁₀的减小趋势更大,说明影响能见度的颗粒物以细粒子为主。平均风速与能见度变化趋势基本一致,与PM_2.5/PM₁₀、PM_1.0/PM₁₀的变化趋势呈反相关。随着雨强的增大,降水日能见度平均值随之减小,降水前一日和后一日的能见度平均值均大于降水日,且降水前一日及后一日的能见度改变量及改变率的绝对值随着降水强度的增加而增加。波长指数的变化说明影响鞍山能见度变化的污染物粒子整体较稳定,能见度与AOD成明显的反相关。     

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。     

2007和2008年夏季北京奥运馆大气PM10与PM2.5质量浓度变化特征

为了监测北京奥运主场馆附近大气颗粒物的污染状况以及评估奥运污染源减排措施对北京大气颗粒物质量浓度变化的影响,利用颗粒物在线监测仪器TEOM于2007年和2008年夏季,在奥运主场馆附近的中国科学院遥感应用研究所办公楼楼顶对大气颗粒物PM10和PM2.5进行了连续同步观测。结果表明,2007年夏季监测点附近大气PM10与PM2.5质量浓度的平均值分别为153.9和71.2μg.m-3,而2008年夏季PM10与PM2.5质量浓度的平均值分别为85.2和52.8μg.m-3。与奥运前一年同时段相比,奥运时段大气PM10和PM2.5的质量浓度分别下降44.5%和25.1%。对比分析奥运前后的2次典型污染过程发现,空气相对湿度的增加和偏南气流输送的共同影响易造成大气颗粒物的累积增长,而降雨的湿清除作用和偏北气流则会使大气颗粒物浓度迅速降低。在相近的气象条件下,奥运前后的污染过程中,大气细粒子的日均增长速率分别为25.1和13.9μg.m-3.d-1,而大气粗粒子的日均增长速率分别为20.8和2.2μg.m-3.d-1,奥运时段污染累积过程中大气粗、细粒子的增长速率分别显著低于和略低于奥运前同时段污染过程中颗粒物的增长速率。污染源减排措施的实施是奥运期间大气颗粒物质量浓度降低的主要原因,从控制效果来看,奥运期间实施的污染源减排措施对大气粗粒子的控制效果明显好于大气细粒子。