Size, composition, and mixing state of individual aerosol particles in a South China coastal city

Aerosol samples were collected in summer in Macao,a coastal city of the Pearl River Delta Region in China.Morphology,size,elemental composition,and mixing state of individual aerosol particles were determined by scanning electron microscopy coupled energy dispersive X-ray(SEM/EDX) and transmission electron microscopy(TEM).Based on the morphologies of 5711 aerosol particles,they consist of soot(32%),mineral(17%),secondary(22%),and unknown fine particles(29%).The sizes of these particles were mostly distributed between 0.1 and 0.4 μm.Compositions of 202 mineral particles were obtained by SEM/EDX.Mineral particles were mainly classified into three types:Si-rich,Ca-rich,and Na-rich.The compositions of typical mineral particles can indicate their sources in sampling location.For example,mineral particles,collected along the main street,were associated with trace amounts of heavy metals,such as Zn,Ti,Mn,Ba,Pb,and As.TEM observations indicate that most Na-rich particles were aged sea salt particles(e.g.,Na2SO4 and NaNO3) which formed through heterogeneous chemical reactions between sea salt and acidic gases.Additionally,aging time of soot was short in Macao due to high humidity,high temperature,and high levels of sunlight in Macao.Most of soot and fine mineral dust particles were internally mixed with secondary particles.     

机动车尾气碳质气溶胶排放因子及其稳定碳同位素特征

机动车尾气是大气碳质气溶胶的重要人为来源,其排放因子与稳定碳同位素组成是重要的基础数据.选取多辆不同类型在用机动车,进行多种工况、冷/热条件下启动的台架试验,收集各测试阶段尾气分析其碳质组分含量与稳定碳同位素比值,并探讨其影响因素.结果表明,总碳排放因子大小为：重型柴油车>轻型柴油车>轻型汽油车,轻型天然气车虽然在低速与中速阶段排放因子极低,但高速行驶阶段可达到重型柴油车的排放水平.各型车冷启动的排放因子均高于热启动,NEDC工况的排放因子整体低于WLTC工况,应与其测试车速有关.汽油车和天然气车各测试阶段排放有机碳(OC)均远高于元素碳(EC),柴油车OC与EC排放因子相近,各类车辆OC/EC都随测试车速的提高而上升.稳定碳同位素EC重于OC,同位素比值大小关系均呈现：汽油车<天然气车<轻型柴油车<重型柴油车,现有源解析的稳定碳同位素源谱较难反映汽油车与天然气车特征.在排放治理与源解析工作中,应注意替代燃料的使用与机动车老化过程所造成的排放因子与同位素特征值的变化影响.     

怠速起停对汽油车油耗及颗粒数量排放的影响

以一辆配置怠速起停系统的国V缸内直喷汽油车为研究对象,使用底盘测功机试验系统、全流稀释采样系统和固态颗粒计数系统,试验研究怠速起停对缸内直喷汽油车油耗与颗粒数量排放的影响,并分析起动温度、试验循环等因素的影响.结果表明,NEDC循环车辆冷机起动时,车辆怠速起停系统开启的百公里油耗降低了5.1%,颗粒数量排放升高了16.7%;车辆热机起动,怠速起停开启产生的百公里油耗降幅增大到7.3%,颗粒数量排放升幅减小至9.3%;WLTC循环热机起动,车辆怠速起停系统开启的百公里油耗降幅减少到1.7%,颗粒数量排放升幅减少到6.2%.怠速起停有利于降低汽车的百公里油耗,但不利于缸内直喷汽油车颗粒数量排放的控制.     

基于低温工况速度变化的CAL3QHC模型修正

我国寒冷地区冬季具有交通拥挤严重、车辆加减速频率和怠速比例高、行驶工况恶劣、排放集中不易扩散等特点。针对上述特点,引入加减速排放参数改进CAL3QHC模型,在低温条件下利用台架实验对各类基础排放率进行修正,并根据实地调查寒冷地区城市道路交通特征修正IVE模型得到NO_x和PM的单车综合排放因子、加速排放因子和减速排放因子。通过对哈尔滨冬季实地调查和车载实验分析,对修正模型NO_x和PM的预测进行检验。研究结果表明,修正后的模型NO_x和PM的相对误差减小了9.2%和19.4%。     

缸内直喷汽油车细小颗粒物排放特性研究

选取三辆满足国六排放标准的缸内直喷汽油车进行常温冷启动WLTC循环排放试验,研究不同车辆排放的粒径在23nm以上的固态颗粒物、6nm以上包含挥发性/半挥发性组分的颗粒物数量排放特性,并进行了比较研究.结果发现,在缸内直喷汽油车排放的6~30nm范围内包含挥发性/半挥发性物质的细颗粒物主要产生在WLTC循环减速段､高速段和超高速段;30~2500nm范围的挥发性/半挥发性的颗粒物主要在超高速段生成;其它工况下,23nm以上固态颗粒物在颗粒物数量排放中占主体.试验研究还发现GPF对6~30nm大小的细颗粒物捕集效果不佳,并且GPF再生时会产生高浓度6~30nm大小的细颗粒物排放.颗粒物碳质成分分析表明挥发性/半挥发性细颗粒物对法规测量的23~2500nm颗粒物的数量排放影响甚微,但对颗粒物质量排放影响明显.     

汽车排放超细微粒数浓度及粒径谱特征的实验研究

采用快速迁移率粒径谱仪(fast mobility particle sizer,FMPS)结合汽车尾气分析仪对3辆不同型号汽车排放超细颗粒数浓度进行测量,分析了空载情况不同转速下排气管附近超细颗粒数浓度及粒径谱特征.结果表明,在怠速800 r·min-1情况下,汽车排放的颗粒数浓度最低,随着空载转速的增加颗粒数浓度呈增高趋势.尾气颗粒以核模态和爱根核模态为主,峰值粒径集中在10 nm和50 nm.汽车加速过程排放颗粒数浓度有明显的急剧升高过程,在车速稳定后颗粒物浓度趋于稳定.在排气管尾部轴向距离0.4 m范围内颗粒稀释后数浓度衰减迅速,在0.4~1 m范围稀释不明显,均大于背景浓度.空载情况下随发动机转速增加,汽车排放尾气CO、HC和NO浓度呈减少趋势,与颗粒物数浓度排放趋势相反.     

The influence of ambient temperature on tailpipe emissions from 1985 to 1987 model year light-duty gasoline motor vehicles—II

Tailpipe emissions from gasoline fieled motor vehicles are sensitive to a number of factors including driving schedule (speed vs time), ambient temperature and fuel composition. The sensitivity of hydrocarbon (HC), aldehyde, CO, and oxides of nitrogen (NO_x) emissions to these variables was examined with 11 recent technology (1985–1987 model year) four- six- and eight-cylinder gasoline fueled motor vehicles. In excess of 200 individual HCs and 12 aldehydes were included in the detailed organic emission characterizations. Two fuels and driving schedules were used. Hydrocarbon and CO emissions increased significantly and NO_x emissions, in general, increased slightly as ambient temperature decreased. Formaldehyde also increased only slightly at test temperature decreased. Paraffin and aromatic emission fractions were dependent on fuel composition with olefin fraction being less fuel sensitive. When the low temperature cold start was preceded by a 5 min engine idle, CO and HC emissions were lowered, and NO_x emissions essentially unchanged.     

Characterization of coal burning-derived individual particles emitted from an experimental domestic stove

Coal combustion in the domestic stoves, which is common in most parts of the Chinese countryside, can release harmful substances into the air and cause health issues. In this study, particles emitted from laboratory stove combustion of the raw powder coals were analyzed for morphologies and chemical compositions by using transmission electron microscopy(TEM) coupled with energy-dispersive X-ray spectrometry(EDX). The coal burning-derived individual particles were classified into two groups: carbonaceous particles(including soot aggregates and organic particles) and non-carbonaceous particles(including sulfate, mineral and metal particles). The non-carbonaceous particles, which constituted a majority of the coal burning-derived emissions, were subdivided into Si-rich, S-rich, K-rich,Ca-rich, and Fe-rich particles according to the elemental compositions. The Si-rich, S-rich and K-rich particles are commonly observed in the coal burning emission. The proportions for particles of different types exhibit obvious coal-issue dependence. Burning of coal with high ash yield could emit more non-carbonaceous particles, and burning of coal with high sulfur content can emit more S-rich particles. By comparing the S-rich particles from this coal burning experiment with those in the atmosphere, we draw a conclusion that some S-rich particles in the atmosphere in China could be mainly sourced from coal combustion.     

满足国六排放的缸内直喷汽油车污染物排放特性试验研究

以满足国六排放的某缸内直喷轻型汽油车为研究对象,试验研究了该车国六Ⅰ型测试循环(WLTC循环)排放的CO、THC、NOx和固态颗粒数量,以及包含挥发性/半挥发性组分的颗粒物数量和粒径分布特性.结果表明:WLTC循环工况覆盖范围广、车速高、加速度大的特点导致污染物排放增加;车辆冷机起动、暖机过程、瞬态过渡工况和高速大负荷工况对车辆的污染物排放影响较大,研发合理的车辆起动、催化剂起燃和暖机热管理策略、提高发动机瞬态过渡工况响应性是控制排放的重点;包含挥发性/半挥发性组分的颗粒物数量排放呈单峰分布,在15 nm附近达到峰值.     

轻型汽油车排放颗粒物数浓度和粒径分布特征

我国机动车颗粒物排放研究多集中于重型柴油车,对于轻型汽油车的研究相对较少.本研究对3辆缸内直喷(GDI)汽车和1辆进气道喷射(PFI)汽车排放颗粒物的数浓度与粒径分布进行测试,并利用两台不同检测下限的颗粒物冷凝生长计数器(CPC)对轻型汽油车颗粒物实际排放水平进行了探究.结果表明,GDI汽车排放的颗粒物数浓度高于PFI汽车一个数量级,冷启动下颗粒物主要在测试循环前200 s大量产生,GDI汽车排放颗粒物数浓度与工况速度变化关系密切,而PFI汽车变化相对较小.GDI与PFI汽车排放的颗粒物粒径分布均具有核模态和积聚模态两个特征峰,核模态颗粒物峰值粒径约为20~27 nm,积聚模态约为80~95 nm.粒径检测下限为2.5 nm的UCPC测得的颗粒物数浓度比法规使用的粒径测量下限为23 nm的CPC测量结果分别高出35.0%(GDI)和50.4%(PFI).表明喷油技术是影响颗粒物数量排放水平的关键因素,法规测试会低估轻型汽油车实际颗粒物排放水平.     

基于TEM-EDS对四川盆地大气单颗粒气溶胶的研究

为了解四川盆地大气中单颗粒气溶胶理化特征,分别在该区域典型城市（成都市）和背景地区（峨眉山）进行了大气单颗粒样品采集.基于带能谱的透射电子显微镜（TEM-EDS）对两地累计3923个单颗粒的化学组成、形貌特征及混合状态等进行了全面观测和分析,并对两地颗粒物差异性进行了对比分析.结果发现：两地气溶胶颗粒主要包括有机物、富硫、矿物、烟尘和飞灰/金属颗粒,除了以单独的外混形式存在外,大多数颗粒以两种及两种以上颗粒类型混合（即内混）形式存在.通过对成都市不同污染状况下单颗粒特征对比发现,"污染天"的内混颗粒占比高于"清洁天",分别为74.2%和68.6%;相比"清洁天","污染天"颗粒物粒径分布范围更广且峰值区间更大,表明污染过程中颗粒物的大气混合趋于更强.对比成都市与峨眉山分析结果得知,成都市以内混的有机物-硫颗粒为主导（占比为50.2%）,而峨眉山以外混的有机物颗粒为主导（占比为50.5%）;成都市含硫类颗粒物（如有机物-硫颗粒）贡献高于峨眉山,而峨眉山两种含碳类颗粒（如烟尘和有机物-烟尘颗粒）占比高于成都市;此外,成都市与峨眉山两地大气颗粒物粒径分布范围及峰值区间均存在一定差异,进一步体现了两地颗粒物来源和老化混合的差异.在峨眉山,与非降雨天相比,一些易溶于水的颗粒物（如含硫类颗粒）在降雨天占比明显降低,而源自当地燃烧过程、粒径较小且疏水性强的颗粒物（如烟尘和有机物-烟尘颗粒）占比相应升高.     

重型柴油车污染物排放因子测量的影响因素

为了调查我国重型柴油车排放污染物的基本水平,确定CO、HC、NO_x和颗粒物等污染物的排放因子,利用满足国Ⅲ排放标准的重型柴油车,分别采用PEMS(portable emission measurement system,车载排放测试系统,由便携式SEMTECH-DS型气态污染物排放测量设备和DMM颗粒物排放测量设备组成)及满足法规排放测量要求的重型车整车底盘测功机方法,研究了不同负载(0%、50%、100%及120%)和2种测试工况对重型车排放因子测量的影响. 结果表明:过载(120%负载)下NO_x和颗粒物等排放因子均比零负载下高出近90%;在平均车速较低、怠速时间长的VECC工况下,气态污染物、颗粒物的排放因子比平均车速高、怠速时间短的C-WTVC工况高出30%左右;PEMS系统和重型车底盘测功机系统所测气态污染物排放因子的相关性较好,但DMM颗粒物排放测试设备与重型车整车底盘测功机所测的颗粒物排放因子相差可达50%左右.      

Oxidation of diesel soot on binary oxide CuCr(Co)-based monoliths

Binary oxide systems(Cu Cr2O4, Cu Co2O4), deposited onto cordierite monoliths of honeycomb structure with a second support(finely dispersed Al2O3), were prepared as filters for catalytic combustion of diesel soot using internal combustion engine’s gas exhausts(O2, NOx, H2 O, CO2) and O3 as oxidizing agents. It is shown that the second support increases soot capacity of aforementioned filters, and causes dispersion of the particles of spinel phases as active components enhancing thereby catalyst activity and selectivity of soot combustion to CO2. Oxidants used can be arranged with reference to decreasing their activity in a following series: O3 NO2> H2 O > NO > O2> CO2. Ozone proved to be the most efficient oxidizing agent: the diesel soot combustion by O3 occurs intensively(in the presence of copper chromite based catalyst) even at closing to ambient temperatures.Results obtained give a basis for the conclusion that using a catalytic coating on soot filters in the form of aforementioned binary oxide systems and ozone as the initiator of the oxidation processes is a promising approach in solving the problem of comprehensive purification of automotive exhaust gases at relatively low temperatures, known as the "cold start" problem.     

2008北京残奥会期间大气黑碳气溶胶污染特征

利用单颗粒黑碳光度计(SP2)对2008年残奥会期间北京市黑碳(BC)气溶胶的质量浓度、粒径分布及单颗粒混合态进行连续在线观测.结果表明:观测期间BC浓度均值为1.65μg/m3,低于往年同期水平;质量粒径分布呈单峰型,峰值位于207nm;内混态BC比例平均为56.1%,高于其他国内外城市,说明本地源排放贡献相对较小.随大气边界层高度及本地源排放变化,BC浓度在上午8:00和午夜0:00出现2个峰值,内混态BC比例日变化趋势与之相反.风向风速分析表明,残奥会期间来自五环外未限行区域的机动车排放对市区BC浓度有明显影响.     

典型城市轻型汽油车尾气排放模式分析

为建立典型城市机动车驾驶模式并量化其尾气排放,研究选取成都市内26辆满足国V排放标准(GB 18352.5-2013《轻型汽车污染物排放限值及测量方法(中国第五阶段)》)的轻型汽油车,利用便携式尾气测量系统测量其现实条件下的行驶工况及尾气排放,并根据实际情况结合分类回归树方法构建本地化的驾驶模式并分析各模式的尾气排放....     

北京市冬季室内空气PM10微观形貌及粒度分布

探讨了北京市吸烟和非吸烟4户家庭室内外空气可吸入颗粒物(PM10)的质量浓度变化规律,利用高分辨场发射扫描电镜(FESEM)和图像分析技术研究了室内PM10的微观形貌特征及粒径分布特点.结果表明,吸烟室内PM10浓度一般高于非吸烟室内;室内PM10一般由烟尘集合体、燃煤飞灰、矿物颗粒、生物质颗粒及未知颗粒共5种颗粒物组成.吸烟和非吸烟室内PM10的粒径一般小于2.5祄,呈双峰分布,其中在吸烟室内,烟尘集合体和未知颗粒等的贡献比较大,而非吸烟室内PM10的数量-粒度分布也为双峰分布,烟尘集合体、燃煤飞灰的贡献比较大.吸烟和非吸烟室内PM10的体积-粒度分布均为单峰分布,并且集中在2.5~10祄范围,其中吸烟室内的烟尘集合体、矿物颗粒物占优势,而非吸烟的室内矿物颗粒占优势.虽然矿物颗粒对粒度粒径的贡献较小,但对体积的贡献比较大.     

怠速条件下汽车排气污染物在排气尾流中扩散特性的实验研究

通过实验的方法对怠速条件下汽车排气污染物在排气尾流中的扩散特性进行了研究.测定了怠速条件下汽车排气尾流中的污染物体积分数及其分布,并比较分析了3种不同类型汽车的污染物排放体积分数及其变化.实验结果表明,怠速时汽车排气尾流中的污染物体积分数按照近似指数函数的趋势迅速降低到接近大气背景值;不同类型汽车排气尾流中的污染物体积分数的差别非常明显;排气方向对汽车排放污染物的扩散及其分布具有重要的影响.研究工作可以为怠速工况下汽车排气污染物对周围环境的影响评价提供更多的有用信息.     

太原市工、商业区PM10中PAHs碳同位素组成及来源

利用中流量大气综合采样仪采集太原市工业区和商业区PM₁₀样品,使用GC/IRMS技术分析了PAHs的δ13C值(碳同位素组成),并根据碳同位素质量平衡计算了煤烟尘和机动车尾气对2类功能区的贡献率. 结果表明:工业区PM₁₀中PAHs的δ13C值在-26.0‰~-24.5‰之间,随环数增加呈贫13C趋势,与煤烟尘δ13C值的变化趋势一致,表明煤烟尘是工业区的一个主要污染源;商业区PAHs的δ13C值在-26.6‰~-26.2‰之间,较工业区显著贫13C,商业区与工业区的污染源有明显差异;除机动车尾气和煤烟尘外,工业区和商业区还有其他污染源输入,其中工业区有生物质燃烧排放输入,商业区有机动车曲轴箱润滑油残渣输入;煤烟尘和生物质燃烧对工业区的贡献率分别为59.3%~70.8%和29.2%~40.7%,表明工业区煤烟污染严重;机动车对商业区PAHs的贡献率在86.1%~95.8%之间,是商业区PM₁₀中PAHs的主要排放源,其中润滑油残渣的贡献率(在40.9%~85.3%之间)最大,机动车尾气的贡献率在8.3%~54.9%范围内,而煤烟尘的贡献率(在4.2%~13.9%之间)最小.      

2011年秋季广州城区大气PM2.5微观形貌和粒度分布

利用高分辨率扫描电镜加能谱仪(SEM-EDX)和图像数据分析技术对2011年秋季广州市中心大气PM2.5的微观形貌和粒度分布特征进行研究,系统获得3种典型颗粒(矿物、烟尘集合体和燃煤飞灰)和其它未知颗粒的数量-粒度分布和体积-粒度分布数据.结果表明,PM2.5颗粒数量-粒度分布峰值落在0.1~0.2μm之间,属于积聚模态中含有气相反应产物的凝结亚模态.3种典型颗粒对PM2.5的数量和体积贡献均为矿物>>烟尘集合体>飞灰.矿物主要分布在0.1~0.3μm范围内,所占数量百分比为41.97%,其中0.1~0.2μm范围内矿物占比高达26.42%,是影响PM2.5颗粒整体分布的主要因素.不同采样时段(上午、下午、晚上)和下雨前后PM2.5颗粒的粒度分布特征基本一致,但晚上和下雨后小于0.1μm的颗粒比例有明显减少趋势.     

生物柴油的碳烟形貌及影响因素分析

使用热场发射扫描电子显微镜拍摄了5种生物柴油和0号柴油在常温常压状态下燃烧产生的碳烟照片,分析了碳烟粒子的形貌及影响形貌和生成量的因素。研究表明,碳烟粒子多呈球状,平均直径在35～75nm之间,粒径分布符合高斯分布,总体排列呈现链状或者块状;碳烟形貌及生成量与火焰温度、燃料的氧含量、芳香烃含量、硫含量以及十六烷值等因素有关,与柴油相比,生物柴油燃烧火焰温度高、含氧量高、芳香烃和硫含量少,十六烷值高,使生物柴油的碳烟粒径普遍较小,整体排列更紧密,粘结程度更强。