Characterization of particles emitted by domestic heating units fueled by distilled oil

Aerosol samples were collected from point sources of different capacity fueled by distilled oil, with the aim of determining the amount and composition of particles emitted by domestic units. A physical and chemical characterization of the particles emitted from each source was performed. Mass median aerodynamic diameter and size distributions were determined. Individual analyses to examine morphology and elemental composition were performed by scanning electron microscopy with an energy dispersive X-ray analyser. The results evidence the specific differences existing in the aerosol emissions of the sources studied in comparison with other combustion sources.     

Dealing with near collinearity in chemical mass balance receptor models

The amount of airborne particulate pollution attributable to various sources can be estimated from a linear least squares (LLS) fit of concentrations of chemical elements observed at a receptor to the known elemental composition of the particles emitted by the sources. The resulting least squares problem often displays a high degree of ill-conditioning and associated inflation of the uncertainties in the estimates. Because of the physical constraints of the problem, variable selection and ridge regression cannot be used to remedy the ill-conditioning. In particular, it is shown that a stable ridge regression solution is equivalent to assuming sources of airborne particulates with negative elemental composition. A method is developed which defines, for a specific level of acceptable uncertainty, three classes of sources; those which can be estimated accurately by LLS, those which cannot be so estimated and those which cannot be accurately estimated individually but participate in linear combinations which can be accurately estimated. A technique is presented which determines those linear combinations of source contributions of minimum variance.     

机动车排放细微/超细颗粒物消光特性的Mie理论研究

机动车等燃烧源排放颗粒物离散系统的消光特性主要取决于颗粒群的物理化学组分和粒径分布特征. 利用内部混合模型,确定典型机动车排放颗粒物的密度和光学复折射系数(m),通过Mie理论模型研究不同粒径下单体颗粒物的光学特性,从而研究机动车排放的nm/μm级粒径下细微/超细颗粒物的无量纲光散射率(Q_scat)、无量纲光吸收率(Q_abs)以及无量纲消光率(Q_ext). 结果表明,不同国家的轻型柴油车(LDV)排放超细颗粒物的化学组分差异较大,而重型柴油车(HDV)则没有显著差别. 相关性分析表明,机动车排放颗粒物的EC组分所占比例与复折射系数的实部(n)和虚部(k)均有极强相关性,相关系数(R>/sup>2)分别为0.995 6和0.993 8.通过Mie理论计算 4种复折射系数下典型机动车排放颗粒物Q_scat,Q_abs和Q_ext随粒径的变化特征发现,粒径为400～600 nm范围的单体颗粒物消光作用最大. 当颗粒物粒径>1 μm时,Q_scat,Q_abs和Q_ext逐渐稳定为常数1.2,1.0和2.2, 此时消光率与复折射系数无关.      

利用SPAMS研究南宁市四季细颗粒物的化学成分及污染来源

为研究南宁市四季大气颗粒物的化学成分及污染来源,利用单颗粒气溶胶质谱仪(single particle aerosol mass spectrometer,SPAMS)对南宁市2015年四季大气细颗粒物进行观测.SPAMS所测得4个观测阶段大气细颗粒物数浓度与细颗粒物质量浓度线性相关系数均在0.75以上,在一定程度上颗粒物数浓度可反映大气污染状况.南宁市四季大气细颗粒物平均质谱图体现出冬、春两季二次反应生成的污染物质较多.利用自适应共振神经网络分类方法对细颗粒物化学成分进行分类,南宁市细颗粒物各化学成分数浓度占比和污染来源在四季均有差异,且化学成分能体现污染来源.冬季元素碳最高,对应较高的燃煤源;秋季有机碳最高,对应较高的机动车尾气源;夏季富钾颗粒、左旋葡聚糖和矿物质较高,对应较高的生物质燃烧源和扬尘源;春季富钠颗粒和重金属略高.在污染升高过程,生物质燃烧源和燃煤源等贡献较大.     

北京餐饮源排放细粒子理化特征及其对有机颗粒物的贡献

调研了北京餐饮业发展现状,通过在线监测、采样分析等手段研究北京4家不同烹调方式的餐馆所排放颗粒物的质量浓度、粒径分布、形貌特征、化学组分,并初步估算餐饮源排放细粒子对北京细粒子中颗粒有机物的贡献.结果表明,餐馆的原料、烹饪过程、油烟去除装置以及客流量都会影响餐馆所排放颗粒物的物理、化学性质.样本餐馆营业期间排放颗粒物PM_{2 .5}质量浓度是当日环境大气PM_{2 .5}质量浓度的8～35倍,PM_{1 .0}在PM_{2 .5}的质量浓度中约占50%～85%.餐饮源排放颗粒物多以固态和液态颗粒物形貌存在,化学组分质量百分数由多到少依次是有机物、无机离子和元素碳,分别占到PM_{2 .5}质量浓度的70%左右、5%～11%和小于2%.初步估计结果表明,北京餐饮源排放细粒子对有机颗粒物的贡献和交通源的排放相当,成为北京细粒子有机颗粒物的主要来源之一.认识餐饮源排放颗粒物的理化性质,可以为改善北京空气质量和保证居民身体健康提供数据支持.     

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.     

循环流化床电站排放烟尘特性及痕量重金属分析

对35t h循环流化床电厂电除尘器入口和出口的烟气气溶胶进行分级取样,得到飞灰浓度和粒度分布以及电除尘器的分级脱除效率.电除尘器对PM10、PM2 5的脱除效率分别为94 34%和91 38%,使部分可吸入烟尘颗粒穿透除尘设备而直接排放到大气环境中.同时对不同粒度飞灰中重金属含量进行了测试,得到痕量元素浓度从高到低依次为Ni,Cr,Cu,Cd,Pb,Hg.痕量重金属含量与飞灰粒径有一定依附关系,其分布规律与煤成分、锅炉燃烧方式和痕量元素自身的挥发特性等因素有关.     

Distribution of rare earth elements in PM10 emitted from burning coals and soil-mixed coal briquettes

Emission from burning coals is one of the major sources of the airborne particles in China. We carried out a study on the rare earth elements (REEs) in the inhalable particulate matter (PM₁₀) emitted from burning coals and soil-coal honeycomb briquettes with different volatile contents and ash yields in a combustion-dilution system. Gravimetric analysis indicates that the equivalent mass concentration of the PM₁₀ emitted from burning the coals is higher than that emitted from burning the briquettes. The ICP-MS analysis indicates that the contents of total REEs in the coal-burning PM₁₀ are lower than those in the briquette-burning PM₁₀. In addition, the contents of the light rare earth elements (LREEs) are higher than those of the heavy rare earth elements (HREEs) in the PM₁₀ emitted from burning the coals and briquettes, demonstrating that the REEs in both the coal-burning and briquette-burning PM₁₀ are dominated by LREEs. The higher contents of total REEs and LREEs in the coal-burning PM₁₀ are associated with the higher ash yields and lower volatile contents in the raw coals. A comparative analysis indicates that the La/Sm ratios in the PM₁₀ emitted from burning the coals and briquettes, being lower than 2, are lower than those in the particles from gasoline-powered vehicle emission.     

Size distribution of particulate polycyclic aromatic hydrocarbons in fresh combustion smoke and ambient air: A review

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous in the atmosphere and they mostly stem from the imperfect combustion of fossil fuels and biofuels. PAHs are inherently associated with homogenous fine particles or distributed to different-sized particles during the aging of air masses. PAHs carried by fine particles undergo a long-range transport to remote areas while those adsorbed on coarse particles have a shorter lifetime in ambient air. More importantly, PAHs with higher molecular weights tend to be bound with finer particles and can deeply enter the lungs, posing severe health risks to humans. Thus, the environmental fate and health effects of particulate PAHs are strongly size-dependent. This review summarizes the size distributions of particulate PAHs freshly emitted from combustion sources as well as the distribution patterns of PAHs in ambient particles. It was found that PAHs from stationary sources are primarily bound to fine particles, which are slightly larger than particles to which PAHs from mobile sources are bound. In ambient air, particulate PAHs are distributed in larger size modes than those in the combustion fume, and the particle size decreases with PAH molecular weight increasing. The relevant mechanisms and influencing factors of particle size distribution changes are illustrated in this article, which are essentially attributed to combustion and ambient temperature as well as the physical and chemical properties of PAHs. Overall, the study on the particle size distribution of PAHs will contribute for a full understanding of the origin, atmospheric behaviors and health effects of particulate PAHs.     

利用单颗粒气溶胶质谱仪研究燃煤尘质谱特征

采用单颗粒气溶胶质谱仪(SPAMS)和再悬浮采样器联用的方式对燃煤电厂烟道气样品和下载灰样品的质谱特征进行测定,并使用颗粒物粒径分级采样仪ELPI测定其粒径分布特征.研究表明,SPAMS监测得到的粒径分布与ELPI结果差异较大,SPAMS对于500 nm以上粒径段检测效果较好;两个样品正谱图中有非常明显的锂、钙、钛、铝等金属组分信号和碳组分信号特征,负谱图中硅酸盐、硝酸盐和硫酸盐等信号比较明显,并且随着粒径的增加碳组分、硫酸盐和硝酸盐等组分对应的信号强度逐渐减弱,而硅酸盐、铝、钙和钛等组分对应的信号强度逐渐增强;对两个样品使用ART-2a聚类获得多个颗粒物类别,分析表明,它们均含有元素碳二次类(硫酸盐和硝酸盐缩写为二次Sec)、有机碳二次类、铝元素碳类、铝钙硅酸盐类和富硅酸盐类等颗粒物类别,并且随着粒径的增加金属硅酸盐颗粒出现频率增大,而含碳颗粒与硫酸盐出现频率降低.但烟道气样品和下载灰样品的质谱特征呈显著差异,下载灰样品更能代表燃煤源真实排放特征.建议在今后建立基于单颗粒质谱固定源成分谱时,应使用单颗粒气溶胶质谱仪在外场进行实测,并使用聚类的方法提取不同粒径段上的源质谱特征,可能会取得更好的效果.     

加热移除废弃聚氨酯硬泡中CFC-11的研究

研究了聚氨酯硬泡在不同温度加热过程中的质量损失、生成的气体成分及硬泡结构变化,并对加热聚氨酯硬泡时所释放的发泡剂CFC-11(CCl3F)进行了测定.结果表明,在80~160℃加热聚氨酯硬泡时,CFC-11的释放速率随温度的增加而增加.将破碎后的硬泡颗粒在160℃下加热,既保证硬泡颗粒不发生热解反应,又使包裹和吸附于硬泡中的CFC-11移除速率最快.在160℃下加热过4mm筛硬泡颗粒1,2,4h后,可分别移除的CFC-11占硬泡颗粒中总量的84.5%、95.5%和96.6%,残余CFC-11则需足够长时间才可移除,而加热释放气体中CFC-11占82%~85%.     

正丁醇对柴油机颗粒组分与形貌特征的影响

为探讨柴油机燃用正丁醇-柴油混合燃料降低颗粒排放的机理,采用热重分析仪与场发射扫描电子显微镜,重点对正丁醇-柴油混合燃料燃烧的颗粒形貌特征进行研究,分析了颗粒的组分、微观结构以及粒径分布随w(正丁醇)的变化规律. 结果表明:正丁醇-柴油混合燃料燃烧的颗粒呈团簇状结构,随着w(正丁醇)的增加,团聚程度逐渐提高,排列结构更加紧密;颗粒的粒径逐渐减小,柴油、B5、B10〔B5、B10是指w(正丁醇)分别为5%、10%的正丁醇-柴油混合燃料〕燃烧的颗粒平均粒径分别为1.43、0.85、0.52 μm;颗粒中的主要成分为碳烟,其质量分数约为60%,随着w(正丁醇)的增加,碳烟和可溶有机物组分的质量分数有所增加,硫酸盐、金属等不易挥发组分以及金属元素的质量分数逐渐减少. 研究显示,添加正丁醇,可促进颗粒转化、改善颗粒的氧化过程,使颗粒向小粒径方向移动;由于颗粒中可溶有机物组分含量增加,因此提高了颗粒在碰撞过程中凝并的概率,致使颗粒的团聚程度增加.      

天津临港石化企业VOCs排放特征及环境影响

为研究化工园区VOCs排放特征及其环境影响,选取天津临港工业区内典型企业A、B、C、D、E进行重点监测,对其有组织、无组织排放各环节、厂界和敏感点的VOCs种类和浓度进行定性和定量分析,并利用偏相关分析方法对其厂界和敏感点进行环境影响因素研究.结果表明,企业A、B、D、E有组织排放的ρ（总VOCs）分别为2.32、1.16、3.30、35.85 mg/m3,其主要污染物分别为环己烷及其同分异构体、丙烯、丙烯腈、甲醇.企业A、B、C、D的无组织排放均以烷烃为主,主要污染物为甲基己烷及其同分异构体、正壬烷;企业E的无组织排放以醇类和烷烃为主,主要污染物为甲醇、正十一烷和乙烷.敏感点的主要污染物与各企业的主要污染物相似.研究显示,企业A、D、E的有组织排放ρ（总VOCs）比无组织大,分别以烷烃、氰化物和醇类为主,企业B、C以无组织烷烃排放为主.无组织排放是影响企业厂界ρ（VOCs）的主要因素;以生产丙烯为主的企业B对敏感点影响最大,相关系数为0.582（P≤0.01）,是影响园区敏感点的主要污染源.      

大气细颗粒物的透射电子显微镜研究

利用透射电子显微镜(TEM)对北京市区和背景点的细颗粒物(PM2.5)的形貌特征和集聚状态进行分析,结合颗粒物能谱(EDX)和选区电子衍射(SAED)特征,将北京市大气细颗粒物分为烟尘集合体、飞灰、矿物颗粒、硫酸盐和有机颗粒等5种单颗粒类型,并讨论了它们的来源.TEM分析表明,北京市区和背景点大气细颗粒物中不同类型的单颗粒所占比例不同,表明市区和背景点细颗粒物的污染物源有所不同.研究还表明,不同类型的细颗粒之间常常发生聚集.     

Sources and composition of aerosol from Khartoum,Sudan

Aerosol sampling was carried out during December 1989 in Khartoum, Sudan, using Nuclepore membrane filters. Twenty-four aerosol samples were collected and analysed by X-ray fluorescence (XRF) spectrometry and particle-induced X-ray emission (PIXE). In addition, individual particle analysis was also performed on 19 samples using electron probe X-ray microanalysis (EPXMA). Good agreement between XRF and PIXE results was obtained for most of the elements. Enrichment factor calculations indicated that soil dispersion is the dominant source for most elements in the aerosol. However, certain elements showed high enrichment factors indicating the presence of anthropogenic sources. From a comparison with available literature data it appeared that the enrichment factors for the enriched elements in the Khartoum aerosol are among the lowest recorded values for urban aerosol. Absolute principal components analysis (APCA) was performed on the data and confirmed the findings from the enrichment factor calculations, i.e. a dominant soil dispersion source and an anthropogenic source for some of the elements. Because of the very limited number of impotant aerosol sources, the data set was reporduced by the APCA model with a reasonable degree of success. Single particle analysis also showed that most of the particles were soil dust. These particles could further be differentiated into alumino-silicates, quartz and CaCO₃ particles. Some of the particles were found to originate from combustion sources. EPXMA gave clues to the process of formation for some of the particles from combustion sources.     

碳质大气颗粒物的扫描质子微探针分析

碳质颗粒物是大气颗粒物的重要组成部分,对全球气候变化、环境质量、人类健康等有重要影响.本研究使用扫描质子微探针对上海两个典型环境监测点的大气颗粒物及7类污染排放源的单颗粒进行了分析.利用微束非卢瑟福弹性背散射谱micro-EBS(non-Rutherford elastic backscattering,EBS)分析了单颗粒中的C含量,发现燃煤烟尘、燃油烟尘、汽车尾气、柴油公交车尾气等污染源中碳质颗粒物占优,而水泥尘、钢铁工业尘、土壤尘中无机颗粒物占优;中心城区的碳质颗粒物占优,而工业区的无机颗粒物占优,单颗粒物的元素分布可以反映颗粒物发生大气化学反应的重要信息,利用微束质子激发X射线荧谱micro-PIXE(particle induced X-ray emission,PIXE)分析得到了大气颗粒物的S、Ca、Fe等元素分布,发现含Ca的碳质颗粒在大气中发生了硫化反应.     

New approaches to characterizing urban air particles in central London

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The role of atmospheric aerosol composition in climate change

The chemical composition of atmospheric aerosols has been investigated. Contributions ofsulfate and soot in aerosols to the atmospheric extinction are studied. Discussions are made on the problems of aerosol emitted from volcano, forest fires in northern China, 1987 and oil field fires in Kuwait, 1991. It is indicated that the changes in concentration, particle size, and chemical composition of aerosol after those events could have impacts on the climate change either regionally or globally and that the impact of aerosol particles on climate change could compensate for some temperature increase caused by greenhouse gases and the increase of surface intensity of ultraviolet radiation due to ozone layer depletion.     

学校食堂、烤肉店PM2.5的微观形貌及粒度分布

使用带能谱的高分辨率场发射扫描电镜(FESEM)和图像分析技术对食堂和烤肉店PM_2.5(细颗粒物)进行微观形貌观察,研究其数量-粒度分布、体积-粒度分布特征. 结果表明:从微观形貌看,PM_2.5主要有矿物颗粒、烟尘集合体、球形颗粒、其他颗粒(生物质、食盐、纤维)4种,其中矿物颗粒有不规则和规则2种形态. 烤肉店的PM_2.5可观察到形成链状的烟尘集合体,而食堂的可观察到更细颗粒组成的链状烟尘集合体.食堂矿物颗粒分别占颗粒物总数和总体积的69.23%、80.13%;数量-粒度分布呈双峰,主要分布在0.2~0.4μm范围内,小于0.5μm的矿物颗粒占颗粒物总数的58.90%;体积-粒度分布呈单峰,集中在在1~2.5μm.烤肉店矿物颗粒和其他颗粒分别占颗粒物总数的45.67%、44.86%;数量-粒度分布主要集中在0.2~0.4μm,小于0.5μm的矿物颗粒占颗粒物总数的39.41%;从体积-粒度分布上看,1~2.5μm内的矿物颗粒体积占颗粒物总体积的比例(32.36%)最大.      

桂林市流动源对大气细颗粒物的贡献研究

在桂林市2013年机动车保有量数据的基础上,参考清华大学开发的中国多尺度大气污染排放清单模型(MEIC)中的排放因子,估算流动源对大气细颗粒物的贡献。结果表明:桂林市区和桂林3大区域的流动源PM_(2.5)排放量分别为71.96和118.87t;按使用的燃料来分,柴油燃料对桂林市区和桂林3大区域PM_(2.5)贡献率较大,分别为94.07%和90.44%;按机动车类型来分,桂林市区和桂林3大区域的流动源PM_(2.5)主要贡献车型均为重型载货车、大型载客车、中型载货车,3大车型PM_(2.5)贡献率之和均超过80%。