北京市春夏季大气气溶胶的单颗粒分析表征

采集了北京市2000年春夏季大气气溶胶样品5个，采用扫描电镜X射线能谱技术分析大气气溶胶单颗粒约2500个。研究结果表明，沙尘期间，矿物尘是最主要的颗粒物种类，非沙尘期间，北京市大气气溶胶中主要检出矿物尘和含硫颗粒物。夏季随着颗粒物污染的加重，含硫颗粒物的数目百分数增加。是北京市大气颗粒物污染的重要特征。重点讨论了Ca-S颗粒、K-S颗粒和Ca-K-S颗粒三类典型含硫颗粒物的化学组成和粒径分布特征。数目可观的Ca-K-S颗粒以及其他硫酸盐颗粒的生成与相对湿度和云量等气象条件相关，这些颗粒物可能是云中过程的产物。减少SO2排放，减少含硫颗粒物，对于控制北京市的大气颗粒物浓度水平具有重要意义。     

碳质气溶胶的放射性碳同位素(~(14)C)源解析:原理、方法和研究进展

碳质气溶胶(或颗粒物)作为大气气溶胶的重要组成,对环境、气候和人类健康造成了巨大的危害。其主要组成成分有机碳和元素碳具有不同的来源特征,且对人类健康和气候系统的影响也具有明显的差异。放射性碳同位素(14C)不仅能定性区分生物源和化石源,还能定量分析不同来源对有机碳和元素碳的贡献比率。重点评述了放射性碳同位素法对气溶胶源解析的技术原理、分离测试方法以及在我国应用的研究进展;最后提出了国内研究应加强的领域和利用放射性碳同位素法研究大气气溶胶的发展趋势。     

南海–东印度洋海域微生物气溶胶空间分布特征

通过走航观测对南海–东印度洋海域的大气细颗粒物(PM_2.5)(共49个)进行采集,使用DAPI染色荧光显微技术获得微生物气溶胶浓度,开展微生物气溶胶在该海域空间分布特征的研究。结果显示,微生物气溶胶浓度范围在2.14×10⁴～5.93×10⁶ cells·m^-3之间,空间分布明显不均衡,即东印度洋>海峡>南海。在东印度洋海域,微生物气溶胶浓度变化幅度较大,以赤道为界,总体呈现北高南低的趋势。微生物气溶胶的粒径主要分布在0.37～2.5μm之间。南海、海峡和东印度洋赤道以北样品中原核生物占比较高,约65%;而在东印度洋赤道以南,真核生物占比则升高至近50%。最后,本研究根据东印度洋海域微生物气溶胶的差异,对其来源开展研究,揭示了海洋生物分布、海洋环境要素以及人为源远距离传输等因素对于开放海域微生物气溶胶浓度的影响。     

沿海地区气溶胶硅的组成、来源及其生态效应研究进展

作为地壳中第二大元素,硅对土壤形成、陆生高等植物和水生浮游植物生长发育以及碳循环有着重要的影响。在气候变化加剧的背景下,硅生物地球化学循环研究变得格外重要。近年来关于陆地和海洋系统的硅循环研究相对成熟,而大气系统中的硅研究明显缺乏。气溶胶是大气中的活跃组分和元素地球化学循环的重要载体。目前关于气溶胶中硅的组成、来源以及部分地区硅沉降负荷的重要程度的认识还不够,制约了对表层地球系统中硅循环的认知。基于当前国内外的研究成果,总结了气溶胶硅的组成及其与其他元素间的耦合关系,综述了新兴的硅同位素在大气颗粒物溯源方面的应用,分析了沿海地区硅长距离传输的生态效应以及硅纳米颗粒对公共健康的影响。总体来说,气溶胶中硅以无机硅为主,部分近海海域气溶胶硅的沉降对于浮游植物生长具有控制作用。未来需要针对气溶胶硅的产生和转化机理、硅沉降及其对生物地球化学循环关键过程的影响以及硅纳米颗粒的毒理效应等方面开展进一步研究。     

不同天气类型广东大气超级站细粒子污染特征初步研究

2012年5月至7月期间,以广东大气超级监测站为观测平台,利用单颗粒气溶胶质谱仪(SPAMS)和其他多种环境监测仪器对大气污染现象进行高时间分辨的长期连续观测。以能见度和相对湿度为参考,将天气类型划分为2次灰霾、1次暴雨和多次晴朗天气过程。观测结果表明,SPAMS捕获的颗粒物数浓度与PM2.5和PM1的相关性(R2)分别达到0.538和0.448,呈现出一定的相关性。大气颗粒物浓度在不同天气条件下,浓度变化较大,其中,灰霾天气下,PM2.5和PM1浓度最大小时均值分别达到0.132 ng/m3和0.094 ng/m3。观测结果表明,粒径处于600~800 nm的细颗粒物对该区域的灰霾形成过程起了最为关键的作用。该地区的大气颗粒物类型主要可分为7种:元素碳(EC)、有机碳(OC)、元素-有机碳混合(ECOC)、大分子有机碳(HMOC)、海盐(Na-K)、富钾颗粒(K-rich)和富铅颗粒(Pb-rich)。灰霾天气,各类型颗粒物数量浓度均有一定程度的增加,其中以EC和K-rich的增加最为明显。分析表明,第一次灰霾主要是由于大气光化学反应起到主导作用,而生物质燃烧又增大了灰霾程度;第二次灰霾过程,生物质燃烧产生的影响更大。     

若尔盖高原土壤和近地表大气气溶胶铅同位素组成测试及示踪研究

若尔盖高原牧场处于中国偏远洁净高海拔地区,大气沉降是污染物主要来源途径之一。由于季风的影响,污染源的辨析较为困难。本文通过多点大气气溶胶不同季节同时采样方式,利用热电离固体同位素质谱仪可有效校正质谱分析中同位素分馏效应的优点,对若尔盖地区土壤和大气气溶胶的铅同位素比值进行精确分析,并结合季风特征对该地区污染物的来源进行解析。结果表明:土壤的208Pb/204Pb比值变化范围为38.79059±0.00194~38.94461±0.00135,206Pb/207Pb为1.18551±0.00002~1.19362±0.00002;大气气溶胶的208Pb/204Pb比值变化范围为37.49571±0.00117~38.48980±0.00105,206Pb/207Pb为1.12894±0.00001~1.16734±0.00001。该地区土壤铅同位素的特征是放射成因铅高,来自于自身天然存在的岩石矿物,与大气污染关系不大;大气气溶胶的铅同位素组成与土壤差异较大,显示为多元混合模式,受到了天然物质和人类活动来源的混合影响,机动车尾气及来自北部(兰州)和西北部(青海、新疆、哈萨克斯坦、俄罗斯)的大气远程运移是若尔盖大气气溶胶及污染物质的主要来源。     

大气气溶胶地球化学研究进展

大气气溶胶地球化学研究进展刘广深，洪业汤（中国科学院地球化学研究所，贵阳５５０００２）关键词大气，气溶胶，生物地球化学循环天然和人为的颗粒物发生过程使低层大气尤其是对流层，成为大气气溶胶的圈层。大气气溶胶在地球表面无时无处不在，对人类生活和自然过程有...     

二次光化学氧化剂与气溶胶间的非均相过程

光氧化剂和气溶胶颗粒物在大气环境中普遍存在,影响着大气氧化能力和气候,威胁着人类健康。而大气光氧化剂与气溶胶颗粒物间复杂的耦合相互作用能产生二次污染物,使得大气污染过程更为复杂,成为国际大气化学研究的前沿和热点课题。挥发性有机物（VOCs）和氮氧化物（NOx）等一次污染物在大气中经过复杂的光化学反应可形成以臭氧（O3）为主的二次光化学氧化剂,并以大气气溶胶为平台发生非均相反应,使大气污染更严重,引起人们普遍关注。二次光化学氧化剂和气溶胶颗粒物之间非均相过程的实验室研究是深入认识这两者间耦合相互作用的关键,实验室研究可以为分析和深入认识外场观测结果提供基础,还能为数值模式模拟研究提供基本参数。概括了大气二次光化学氧化剂的形成过程,总结了国际上近年来二次光化学氧化剂与大气气溶胶颗粒物非均相反应的实验室研究进展以及研究方法,最后提出了现有的一些主要科学问题,对未来这一重要领域的研究前景进行了展望。     

天山乌鲁木齐河源1号冰川大气气溶胶的微观形貌及元素组成分析

为研究冰川区大气气溶胶单颗粒物的物理化学特征,使用带能谱的扫描电镜(SEM-EDX)对2007年在天山乌鲁木齐河源1号冰川东支积累区海拔4 130m(86°49′E,43°06′N)处采集的38个气溶胶样品中的38 861个单颗粒物进行了微观形貌和元素组成的分析.结果表明:天山乌鲁木齐河源1号冰川区大气气溶胶主要以粒径在0.6～2.5μm之间的不规则的非圆形矿物颗粒为主,其中以富含Si、Ca的粘土矿物颗粒为主,与人类活动密切相关的含S颗粒物及烟尘飞灰等含量较少.这与其它沙尘源区的气溶胶特征相似,其中含Ca颗粒多于其它沙尘源区,主要受西风带的影响.气团轨迹显示,来自于西面中亚地区的高空气流影响了1号冰川区的大气环境,表明天山乌鲁木齐河源1号冰川区的气溶胶主要代表了中亚沙尘源区对流层中上部大气的本底状况.     

青藏高原大气气溶胶研究进展

大气气溶胶是地球大气成分中含量很少的组分之一, 但其对气候环境以及人类健康有着极其重要的影响. 由于青藏高原地理单元的独立性和特殊性, 该地区气溶胶特征和行为的研究引起越来越多的关注.回顾了青藏高原大气气溶胶研究的历史和分析监测方法, 从气溶胶的基本特性、 气候效应、 环境效应三个方面综述了20世纪90年代以来青藏高原大气气溶胶研究的成果, 并对该地区研究的前景有所展望.     

大气气溶胶密度观测研究进展

大气气溶胶的气候效应、环境效应、健康效应均与其物理化学性质密切相关,其中,密度是大气气溶胶重要的物理性质之一。密度影响着粒子的输送过程和在人体肺部的沉积过程。密度可以分别将电迁移率粒径和空气动力学粒径,数浓度和质量浓度联系起来。密度的变化可为气溶胶的形成和老化过程提供信息,细粒子分粒径的密度还可为大气过程和化学组分的演化提供参考依据。因此,研究大气气溶胶密度对了解气溶胶化学组分,评估气溶胶形成过程以及探究气溶胶在人体内的沉积效率具有重要的意义。由于国内在该领域研究总体较少,对大气气溶胶密度的定义、研究方法、国内外研究进展以及影响因素和变化特征等进行较为系统的总结,对未来开展大气气溶胶密度的观测和研究十分必要。     

Studies on aerosol properties during ICARB-2006 campaign period at Hyderabad,India using ground-based measurements and satellite data

Continuous and campaign-based aerosol field measurements are essential in understanding fundamental atmospheric aerosol processes and for evaluating their effect on global climate, environment and human life. Synchronous measurements of Aerosol Optical Depth (AOD), Black Carbon (BC) aerosol mass concentration and aerosol particle size distribution were carried out during the campaign period at tropical urban regions of Hyderabad, India. Daily satellite datasets of DMSP-OLS were processed for night-time forest fires over the Indian region in order to understand the additional sources (forest fires) of aerosol. The higher values in black carbon aerosol mass concentration and aerosol optical depth correlated well with forest fires occurring over the region. Ozone Monitoring Instrument (OMI) aerosol index (AI) variations showed absorbing aerosols over the region and correlated with ground measurements.     

大气微纳米颗粒物界面反应与矿物协同演化意义

综述了大气气溶胶颗粒物的特征、颗粒物的界面反应与矿物协同演化意义;重点介绍了大气颗粒物粒径分布和矿物成分,以及常见有毒有害气体的界面反应产物特征与关键化学过程;总结了矿物颗粒在大气气溶胶形成过程中汇聚、调控、催化的作用,以及颗粒物与大气中SO₂、NO_x的协同反应机制;分析了微纳米颗粒对二次有机气溶胶形成的影响,以及大气矿物相颗粒界面反应产物组合及协同演化作用.可为进一步研究大气颗粒物与大气中痕量污染气体反应形成二次气溶胶进而影响大气化学组成的过程提供指导,对深入探讨大气矿物颗粒表面特性在复合污染物中多介质反应的微界面化学过程,矿物尘-污染物气溶胶体系在雾-霾形成、转换、新生粒子和阻断行为的复合作用具有重要的环境学意义.      

Characterization of indoor and outdoor atmospheric pollutants impacting architectural monuments: the case of San Jerónimo Monastery (Granada, Spain)

Indoor and outdoor concentrations of atmospheric gaseous pollutants as well as composition, size, and morphology of particulate matter have been investigated at the monastery of San Jerónimo in Granada (Southern Spain). Complementary micro- and nano-analytical techniques were applied; elemental and mineralogical composition and morphological characteristics of particulate matter were investigated combining electron probe microanalysis at the single particle level, and bulk aerosol samples were analyzed using energy-dispersive X-ray fluorescence, X-ray diffraction, scanning electron microscopy with energy-dispersive X-ray analyzer and transmission electron microscopy (TEM). Microclimatic conditions at the monastery were monitored, and gas concentrations were assessed by means of diffusion tubes subsequently analyzed with ion chromatography. Results revealed high abundances of soil dust particles (aluminosilicates, calcite, dolomite, quartz), salt aerosols (chlorides, sulfates and ammonium-rich salts), and NO₂ and SO₂ both outdoors and indoors. Amorphous black carbon particles had surprisingly high abundances for Granada, a non-industrialized city. The composition of indoor particles corresponds to severe weathering affecting the construction materials and artworks inside the church; moreover their composition promotes a feedback process that intensifies the deterioration. Chemical reactions between chloride-rich salts and pigments from paintings were confirmed by TEM analyses. Indoors, blackening of surface decorative materials is fostered by particle re-suspension due to cleaning habits in the monastery (i.e. dusting). This is the first air quality study performed in a monument in the city of Granada with the aim of developing a strategy for preventive conservation.     

Experimental data on SOA formation from mixtures of anthropogenic and biogenic organic compounds

Secondary organic aerosols (SOA) constitute a significant fraction of the atmospheric particulate matter. Theses particles are formed as a consequence of the oxidation reaction of certain organic gases that leads to the formation of low-volatility compounds. As for other pollutants, air quality models allow the simulation of particle levels and thus models constitute a powerful tool in air quality management. Nevertheless, the accepted use of models must be based on the validation of its capacity to reproduce observed concentrations. Air monitoring sites provide measured information of a large variety of ambient pollutants. Unfortunately, measurements on SOA are not normally available, as current monitoring networks do not include instrumentation to distinguish primary from secondary sources of organic carbonaceous aerosol. This paper presents a set of photooxidation experiments performed in the European Photorreactor (EUPHORE) smog chamber (CEAM, Spain) under different experimental conditions to investigate SOA formation. The use of chambers allows the isolation of atmospheric chemistry and aerosol formation processes. Thus, although these measurements were obtained at initial precursor concentrations higher than those in atmospheric conditions, they constitute a valuable set of information for SOA model evaluation purposes.     

大气有机氮沉降及其对海洋生态系统的影响

有机氮是大气中含氮物质的重要组成部分。大气中有机氮化合物的种类繁多,按其存在的形态可分为：氧化型、还原型以及生物/颗粒型有机氮,这些有机氮可来自自然源和人为源的直接释放,也可来自于无机氮与碳氢化合物间的大气化学反应。大气有机氮对海洋的输入不仅可以促进海洋初级生产力的增长、进而增加二氧化碳的吸收速率,还可能影响海洋生态系统的结构和功能。分析了海洋大气有机氮沉降的最新研究进展,结果表明：气溶胶中的有机氮在总氮中所占的比例为39.6%±14.7%;陆地雨水中以有机形式存在的溶解氮为30.2%±15.0%,而海洋上,溶解有机氮可达到雨水中总氮的62.8%±3.3%。可见,目前仅包括无机氮沉降的入海通量可能低估了1/3。因此,开展大气有机氮沉降的研究,有助于评价有机氮在全球氮循环中的作用,以及对海洋生态系统的短期和长期的影响。     

Variations in sulphate aerosols concentration during winter monsoon season for two consecutive years using a general circulation model

During the field cruises of the Indian Ocean Experiment (INDOEX) extensive measurements on the atmospheric chemical and aerosol composition are undertaken to study the long-range transport of air pollution from south and southeast Asia towards the Indian Ocean during the dry monsoon season in 1998 and 1999. The present paper discusses the temporal and spatial variations in aerosols and aerosol forcing during the winter monsoon season (January-March) for INDOEX first field phase (FFP) in 1998 and INDOEX intensive field phase (IFP) in 1999. An interactive chemistry/aerosol model (LMDZ.3.3) is used to investigate the variation in the spatial distribution of tropospheric sulphate aerosols during 1998 and 1999. The model results depict major enhancement in the sulphate aerosol concentrations, radiative forcing (RF) and optical depth over the Indian subcontinent and adjoining marine areas between INDOEX-FFP and IFP. A significant increase in transport of sulphate aerosols from the continents to the Indian Ocean region has also been simulated during the winter monsoon in 1999. The mean RF over INDOEX-FFP in 1998 is found to be ?1.2 Wm^–2 while it increased to ?1.85 Wm^–2 during INDOEX-IFP in 1999. Model results reveal a mean sulphate aerosol optical depth (AOD) of 0.08 and 0.14 over Indian subcontinent during 1998 and 1999, respectively. The model results suggest that elevated AOD downwind of source regions in India can significantly affect the regional air quality and adjoining marine environments.     

Sedimentary matter and organic compounds in the aerosols and surface waters along the Transatlantic section

Concentrations and composition of suspended particulate matter and organic compounds (OC), including Сorg, lipids, hydrocarbons (HC), and pigments, were determined in the near-water aerosol layer and in surface waters on the meridional section across the Atlantic Ocean from the port of Ushuaia to the port of Gdansk (Cruise 47^th of the R/V Akademic Ioffe, March 26–May, 7, 2015). It was established that the distribution of OC (except for pigments) in aerosols, in general, repeats the distribution of particle number and weight concentrations of aerosols, with maximums in the influence zone of fluxes from Patagonia and African deserts. The concentrations of aerosols changed within wide ranges: from 1237 to 111739 particles/L for 0.3–1 μm fraction; and from 0.02 to 19.890 μg/m³ for aerosols collected by network method (flux of 0.02–34.4 mg/m² day). The contrasting mineral composition of aeolian material reflects the diversity of its provenances. In surface waters, the studied compounds were accumulated in the frontal river–sea area (runoff of the Rio-Colorado River) and with approaching the coast, especially in the English Channel. A simultaneous change of concentrations of suspended particulate matter and OC is observed only in open oceanic waters.     

A study of water-soluble inorganic ions in size-segregated aerosols in atmospheric pollution episode

Particulate matter, the main pollutant in the atmospheric environment of the Santiago city in winter, was analyzed by means of the major water-soluble ionic species obtained under critical episodes of pollution in 2003. The particulate matter samples were collected using the Micro-Orifice uniform deposit impactors, with eight impactor stages connected in series, and the ionic species in particulate matter samples at each stage was analyzed by ion chromatography. While sulfate ion and nitrate ion showed bi-modal distributions, peaking in the fine and coarse mode, ammonium ion displayed a bi-modal size distribution, peaking in the fine and ultra fine mode. The equivalent concentration ratio of ammonium to sulfate was 2.03 ± 0.09, indicating the complete neutralization of sulfuric acid by ammonia. The excess ammonium ion was associated to nitrate ion. The study of the size distribution of water-soluble inorganic ions in particulate matter supports the notion that secondary aerosols play a significant role in the urban atmosphere.