青藏高原气溶胶单颗粒类型及粒度分布

应用场发射扫描电镜(FESEM)对青藏高原纳木错综合观测站和香格里拉本底站2011年7～8月份不同天气情况下收集的气溶胶样品进行研究。结果表明,区域内气溶胶单颗粒类型主要包括烟尘集合体、球形颗粒(焦油球、燃煤飞灰)、似球形颗粒、矿物颗粒、生物颗粒等,香格里拉的球形颗粒中出现了飞灰颗粒,而纳木错样品中没有。纳木错气溶胶颗粒的数量-粒度峰值和体积-粒度峰值分别出现在0.2～0.3 μm和1～2.5 μm,矿物颗粒数量和体积最多,分别占44.4%和61.7%。香格里拉气溶胶颗粒的数量-粒度峰值和体积-粒度峰值都呈现双峰分布,主峰均分布在>2.5 μm范围,矿物颗粒数量和体积最多,分别占51.7%和58.7%。细粒子和粗粒子分别为纳木错和香格里拉气溶胶的主要类型。纳木错气溶胶中矿物颗粒最多,数量百分比为44.4%,其次为烟尘集合体(29.5%)和球形颗粒(26.1%),香格里拉气溶胶中矿物颗粒数量百分比为51.7%,其次为球形颗粒(29%)和烟尘集合体(19.3%);纳木错气溶胶总颗粒物主要分布在0.2～0.3 μm粒径范围中,数量百分比为32.59%,其中矿物颗粒最多(15%),其次为球形颗粒(11.5%)和烟尘集合体(6.1%)。香格里拉气溶胶颗粒物主要分布在>2.5 μm粒径范围中,数量百分比为37.5%,其中矿物颗粒最多(17.9%),其次为球形颗粒(10%)和烟尘集合体(9.6%)。     

拉萨市夏季大气降尘单颗粒矿物组成及其形貌特征

应用带能谱的电子扫描电镜(SEM-EDX)对拉萨市夏季正常天气下收集的大气自然沉降气溶胶样品进行分析,研究了拉萨市大气降尘矿物组成和各种物相形貌特征信息。拉萨市大气颗粒物含有硅酸盐颗粒、富钙颗粒、富铁颗粒、富碳颗粒(燃煤飞灰颗粒和燃油飞灰颗粒)和植物残体颗粒。根据颗粒物数量统计发现拉萨市大气颗粒物以硅酸盐颗粒为主,富钙颗粒和富铁颗粒次之,需要指出的是以燃油飞灰为主的富碳颗粒已占到一定比重,说明以燃油为主的机动车尾气对拉萨大气污染在加强。研究结果表明,大气降尘矿物成分及其形貌特征可以用作判定污染物来源的重要标志,拉萨大气中颗粒来源的多样性决定了治理措施也应综合进行。     

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.     

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。     

南昌市降尘颗粒物形貌特征和来源电子探针研究

利用电子探针对南昌市降尘颗粒物的形貌特征和成分进行了分析,并探讨了它们的来源.得出南昌市降尘颗粒物的主要组成为矿物颗粒、钙质颗担以及块状烟尘集合体和燃煤飞灰颗粒.不同功能区的采样点颗粒物的组成有一定差异,表明颗粒物的来源不同.根据颗粒物的来源和分布特点,认为南昌市的城市规划布局不甚合理,尚需进一步改善.     

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.      

北极黄河站秋季气团传输影响下大气气溶胶数谱分布特征

2013 年9月在北极黄河站开展了气溶胶数谱（10~400nm）的短期观测实验。数浓度小时平均值主要出现在300~400cm^-3,平均值为350cm^-3,高于新奥尔松Zeppelin 全球大气本底站及环北极海洋大气7-9月航测报道的浓度。大气气溶胶的三个模态（核模态、爱根核模态和积聚模态）数浓度平均分别为35、122和193cm^-3。观测期间没有发生新粒子生成事件,平均数谱分布呈现双模态的分布特征,模态峰值分别出现在30nm和115nm,由积聚模态主导。平均数谱分布的几何中值粒径出现在约100~110nm。从单颗粒分析结果来看,观测期间黄河站地区大气气溶胶主要以海盐气溶胶为主,但是在来自挪威海域和北欧大陆的气团影响下,也观测到煤烟颗粒、富硫颗粒物和含碳颗粒物等人为气溶胶。     

2013年1月京津唐地区霾事件气溶胶单颗粒形貌及硫酸盐化特征

2013年1月华北地区经历了重霾过程,为研究其污染特征,使用透射电子显微镜(TEM)及能谱(EDX)对北京、唐山和天津晴天和霾天气下气溶胶单颗粒基本形貌和硫酸盐化特征进行了分析。结果表明,华北地区气溶胶单颗粒包括矿物颗粒、硫酸盐颗粒、金属氧化物、烟尘集合体、有机颗粒和飞灰,仅在天津市样品中发现少量的Na Cl颗粒。对单颗粒的元素组成进行统计表明,华北地区晴天以富Si颗粒为主(31.0%),其次为富Ca颗粒(18.3%)、富Fe颗粒(14.1%)、富Cl颗粒(12.2%)等,霾天以富S颗粒为主(47.4%),其次为富Si颗粒(21.1%)和富Fe颗粒(13.4%)等。霾天气富Ca颗粒明显减少,同时在含S较高的颗粒中也含有Ca、K等元素,说明大气中含Ca、K等碱性矿物对雾水酸性有一定的缓冲作用。不同天气含S颗粒差异较大,霾天气明显高于晴天,S/Ca平均值在霾天明显较高,且大于0.8,说明在一定的SO2浓度下,大气湿度越大,硫酸盐化现象越明显,生成大量的硫酸铵盐。     

兰州市一次沙尘暴期间PM10的矿物组成特征

为研究兰州市2006年3月31日沙尘暴期间及之前大气PM10中的矿物学特征,运用场发射扫描电镜和带能谱的扫描电镜识别和统计了PM10中单个颗粒的微观形貌特征和矿物组成.结果表明,沙尘暴期间PM10的质量浓度是一个突增渐降的过程,沙尘暴到来时,PM10的质量浓度在短时间内增至约1500 μg/m3,然后随着沙尘暴的消退逐渐降低,在较长时间内保持较高的浓度值,期间主要为矿物颗粒;沙尘暴之前,PM10的质量浓度普遍高于国家二级标准(150 μg/m3),最高可达500 μg/m3,主要颗粒类型有燃煤飞灰、烟尘集合体和少量的矿物颗粒.单颗粒矿物分析表明,沙尘暴之前的非沙尘暴期,单个矿物颗粒的数量百分比从大到小依次为方解石、石英、伊利石、绿泥石、伊/蒙混层、钙长石、钠长石、钾长石、高岭石和石膏等,沙尘暴期间,矿物颗粒中伊利石和绿泥石的数量百分比明显增加,而方解石含量明显减少.     

我国北方冬季灰霾主要有机单颗粒类型及耐热性

我国北方冬季气溶胶中有机物所占比重大,对其气候效应、人体健康及大气环境影响进行评估是大气化学研究的热点问题。为了探究冬季灰霾主要有机单颗粒类型及耐热性,本研究利用透射电镜发现北方冬季灰霾中一次有机颗粒较为普遍,根据内混颗粒物的化学组分差异将其分为三种:有机物–矿物颗粒(3%)、有机物–烟尘颗粒(16%)和有机物–二次无机盐颗粒(81%)。此外,本研究还使用管式炉对采集的大气单颗粒样品进行高温加热,再利用透射电镜对加热后的几类典型有机单颗粒形貌和组分特征进行原位跟踪分析。结果显示,近圆形一次有机物经过300℃和500℃加热过程之后,形貌特征无明显变化,表明该类一次有机颗粒具有耐高温特性;半透明穹顶状有机物在300℃下粒径增大且颜色更加透明,表明在此温度下该类颗粒中大部分有机组分能够挥发;将具有有机包裹层的颗粒物在室温及300℃下的形貌特征对比测量,发现虽然二次有机包裹层留有部分痕迹,但是大部分已挥发,进一步升温至500℃时,半透明穹顶状的有机物和有机包裹层在高温过程中挥发完毕。本研究证明北方冬季燃煤排放的圆形一次有机物含有大量的难挥发耐热有机组分,外场观测和实验室分析应考虑此类一次有机颗...     

煤矿区城市矿物气溶胶的SEM-EDX特征分析

采集煤矿区城市义马、平顶山、永城夏季大气PM₁₀样品,采用带能谱的扫描电镜(SEM-EDX)研究了PM₁₀中的矿物颗粒组成、成因及来源。结果表明,矿区矿物颗粒按化学成分共有5种主要类型,分别为"富Si"、"富Ca"、"富S"、"富K"、"富Cl"型。其中平顶山地区"富Si"颗粒占百分比最高(78%),矿物颗粒硫酸盐化程度小;永城地区硫酸盐化程度中等,几乎所有的"富Ca"碱性碳酸盐颗粒都硫酸盐化成石膏;义马地区矿物硫酸盐化程度最大,除石膏以外,还有一定量硫酸铵形成。永城和义马地区还出现了一定量的"富K"(12.7%)和"富Cl"(10.6%)颗粒,与秸秆焚烧活动有关。通过对3个矿区城市PM₁₀硫酸盐化程度对比可以发现,偏碱性的碳酸盐矿物、煤炭燃烧和秸秆焚烧燃烧释放出大量的酸性SO₂以及较高的空气湿度,均有利于硫酸盐化的进行,硫酸盐颗粒的形成对煤矿区城市的区域性气候具有一定影响。     

Changes in physical and chemical properties of three soil types in India as a result of amendment with fly ash and sewage sludge

The use of coal fly ash and domestic sewage sludge in agriculture is being considered as one of the methods for recycling of these wastes in an environmental beneficial manner. Mixtures with soil were prepared at different proportions of fly ash and sludge, either alone or in combination at a maximum application rate of 52 t ha^-1. The changes in the selected properties and heavy metal contents of three soil types in India were studied after incubating the respective mixtures for 90 days at near field capacity moisture level. Sewage sludge, due to its acidic and saline nature, high organic matter and heavy metals content, had more impact on soil properties than the fly ash. Sludge application produced several changes including an increase in available nitrogen, organic carbon, salinity and water-holding capacity of the soils. The concentrations of major cations and heavy metals also increased because of the sludge application and the pH was decreased. However, the levels of individual metal concentrations in all the mixture types were below the allowable limits prescribed by several environmental agencies. Using fly ash either alone or in equal quantity with sewage sludge had little influence on soil properties and heavy metal content. The relative availability (RA) of heavy metals in three soils amended with 52 t ha^-1 of sewage sludge was observed to be highest in oxisol, followed by alfisol and vertisol.     

华能南京电厂不同粒径粉煤灰中微量元素分布及其富集规律

华能南京电厂不同粒径粉煤灰的化学成分和矿物相组成基本相同，煤粉所含矿物质在高温燃烧过程中的挥发－凝聚作用，导致微量元素趋向细粒径粒煤灰中富集，其富集的程度则与粉煤灰的平均粒径和元素的地球化学性质密切相关，粉煤灰排放的环境效应表明，尤以细粒径灰粒的影响最大。     

季节冻土地区路基冷阻层温度场效应

为研究季节冻土地区冷阻层的路基温度场效应,基于ANSYS软件热分析原理,以粉煤灰土、橡胶颗粒改良粉煤灰土和聚丙烯纤维改良粉煤灰土3种冷阻层材料为研究对象,模拟季节冻土地区道路路基温度场,研究其阻止热量交换的效果。结果表明：采用粉煤灰土为冷阻层的道路的最大冻深为1.32 m,温度梯度最低值为-17.606℃/m;采用橡胶颗粒改良粉煤灰土为冷阻层的道路的最大冻深为0.94 m,温度梯度最低值为-23.563℃/m;聚丙烯纤维改良粉煤灰土为冷阻层的道路的最大冻深为1.20 m,温度梯度最低值为-19.557℃/m。橡胶颗粒改良粉煤灰土冷阻效果最佳,其确保路基土处于零上温度不冻结状态的最小摊铺厚度为0.33 m,适宜作为季节冻土地区的冷阻材料。     

Characterization of fly ash from a power plant and surroundings by micro-Raman spectroscopy

Fly ash samples were collected from a Portuguese power plant that burns low-sulphur coals from South Africa, U.S.A., Colombia, and Australia. The fly ashes were collected from the hoppers of the economizers, air heaters, electrostatic precipitators, and from the stack. The power plant air monitoring system was also sampled. The fly ash characterization was conducted by micro-Raman spectroscopy (MRS). The micro-Raman spectroscopic analysis permitted an efficient identification and characterization of different inorganic and organic materials present in fly ash: quartz, hematite, magnetite, calcite, glass, aluminium and calcium oxides, and different types of organic constituents.The study of the structural evolution of the unburned carbon/char material during their path through the power plant, though the use of Raman spectra and Raman parameters reveal that despite the high temperatures they reached, these materials are still structurally disordered. However, a structural evolution occurs in the char from the economizer up to the electrostatic precipitators where the char is structurally more disordered.The different features of the Raman spectra observed for carbon particles collected from the stack, together with the high range of variation of the Raman parameters, confirm the existence of different carbon particles in the stack, i.e., char and others (probably soot).The filters from the surroundings contain a variety of carbon particles with Raman parameters different from the ones obtained in the fly ash hoppers and stack. These are diesel particles as indicated by the values of W_D1, FWHM_D1, FWHM_G, W_G and ID1/IG obtained.     

Particle size distribution and dissolution properties of metals in cyclone fly ash

The particles in the examined cyclone fly ash were all smaller than 0.25 mm. in diameter, and particles smaller than 0.075 mm. in diameter accounted for 88.4 % of the ash weight. This result indicates that cyclone fly ash consists of particles with a small diameter. The metals in the cyclone fly ash were enriched in small particles. The highest concentrations for zinc, copper, lead, cadmium and molybdenum in the cyclone fly ash were found in the smallest particle size fraction (< 0.075 mm.) and for Barium, chromium, nickel, Vanadium and Cobalt in the second to smallest particle size fraction (0.075-0.125 mm.). From an environmental and toxicological standpoint, the smallest particles are of the greatest concern when ash is handed at landfill disposal sites (transport and disposal especially in stormy weather conditions), and some studies have reported risks to workers from prolonged exposure to ash. The results of the comparison of various dissolution methods for metals showed that the digestion procedures with nitric acid alone (USEPA 3051) or with a mixture of nitric acid + hydrogen peroxide (USEPA 3050B) slightly underestimated the metal concentrations in the cyclone fly ash. Although the use of hydrofluoric acid is often necessary for the determination of a number of elements associated with siliceous minerals, its use can result in loss of trace elements during dissolution.     

Partitioning of major and trace inorganic contaminants in fly ash acid mine drainage derived solid residues

Acid mine drainage was reacted with coal fly ash over a 24 h reaction time and species removal trends evaluated. The evolving process water chemistry was modeled by the geochemical code PHREEQC using WATEQ4 database. Mineralogical analysis of the resulting solid residues was done by X-ray diffraction analysis. Selective sequential extraction was used to evaluate the transfer of species from both acid mine drainage and fly ash to less labile mineral phases that precipitated out. The quantity of fly ash, volume of acid mine drainage in the reaction mixture and reaction time dictated whether the final solution at a given contact time will have a dominant acidic or basic character. Inorganic species removal was dependent on the pH regime generated at a specific reaction time. Sulphate concentration was controlled by precipitation of gypsum, barite, celestite and adsorption on iron-oxy-hydroxides at pH > 5.5. Increase of pH in solution with contact time caused the removal of the metal ions mainly by precipitation, co-precipitation and adsorption. PHREEQC predicted precipitation of iron, aluminium, manganese-bearing phases at pH 5.53–9.12. An amorphous fraction was observed to be the most important in retention of the major and minor species at pH > 6.32. The carbonate fraction was observed to be an important retention pathway at pH 4–5 mainly due to initial local pockets of high alkalinity on surfaces of fly ash particles. Boron was observed to have a strong retention in the carbonate fraction.     

高掺量粉煤灰固结材料的矿物组成及微观结构研究

采用化学成分、X衍射和电子显微镜分析等方法研究了高掺量粉煤灰固结材料的矿物组成及微观结构。结果表明 ,其矿物组成主要是 3Al2 O3 ·2SiO2 和硅铝酸盐的胶凝物相 ,具有较大孔径的多孔结构特征 ,与水泥混凝土的矿物组成和微观结构有较大不同 ;粉煤灰的掺量、养护龄期对水化产物的生成量有直接影响 ;固结剂掺量大于 2 0 %时 ,粉煤灰和固结剂全部反应形成多孔状的胶凝体水化产物