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中国几个城市低对流层大气颗粒中类脂质的特征及其环境有机地球化学意义
张健
1990
学位授予单位中国科学院地球化学研究所
学位授予地点中国科学院地球化学研究所
学位名称博士
学位专业有机地球化学
摘要目前,国际上在环境有机地球化学领域对大气气溶胶的研究仍然处于一个较低的水平。国内这方面的工作更是处于空白。本文针对目前国内亟待解决的与煤、石油有关的能源污染问题,应用有机地球化学和石油地球化学中的一些概念和指标,如同系列化合物的分布、碳优势指数(CPI)、最大主峰碳(Cmax)和分子标志物等,首次系统讨论了我国一些城市大气气溶胶的类脂质(可溶有机质)组成,来源和在空间的分布。提出了如何识别各种能源在使用和贮存中对大气环境造成的污染;同时也提出了这些污染物在我国不同地区(例如,沿海和内地),不同气候带(例如,北方和南方)中的分布规律,以及高度、季节等因素对大气污染的影响。这对于认识我国大气污染的严重性及其影响因素具有重要的参考意义。研究中采用标准过滤式空气采样器一共收集了28个大气尘埃样品。这些样品分别来自北京、广州、贵阳和水城的市区和郊区,其中包括一些象焦化厂、炼油厂和轮胎厂这样的点源样品和背景样品。将所有被收集到的尘埃样品用有机溶剂进行超声抽提后,经甲酯化和硅醚烷化处理,薄层色谱分离可将这些样品的类脂质分为烃类、脂肪酸甲酯、醛酮和脂肪醇四个组分。最后通过GC和GC/MS完成这些组分的化合物分子结构鉴定。用环境有机地球化学方法处理这些分析结果表明:(1)不同点源和背景气溶胶样品的类脂质组成与它们的采样环境之间关系密切,点源气溶胶样品的类脂质组成突出地反映了人为成因的特征,在背景气溶胶中类脂质组成主要代表了生物成因的特征,研究发现煤特别是烟煤的燃烧产物中含有较多杂环芳烃及其氧化产物,而车辆排放物和石油裂解过程中排放的副产物则含有较多三萜烷,一些直接由未燃烧石油产品输入的气溶胶的突出特征表现在样品中具有完整系列的烷基苯化合物;(2)我国四个城市大气气溶胶的类脂质都包含有正烷烃、正脂肪酸、正脂肪醇、多环芳烃、倍半萜、二萜和三萜烷以及甾烷等化合物,这些化合物包括天然生物成因、地质成因和人为成因这三个来源,并按不同的比例进行掺和。不同城市气溶胶的类脂质组成反映了该地区的工业发展水平、交通发达状况、人口密度和地理环境的差别,北京地区气溶胶的类脂质组成反映了我国北方平原地区的特征,广州地区气溶胶的类脂质分布表现了沿海地区的特点,贵阳和水城地区大气尘埃类脂质则代表了我国西南山区的大气污染状况,一般地在城市郊区大气所受到人为污染程度均低于市区;(3)采样高度对气溶胶类脂质的组成和同系列化合物的分布有明显的影响,随着采样高度的增加生物成因组分的比例明显增加,气溶胶的类脂质产率随采样高度增加有明显的重力分异现象;(4)季节将会使气溶胶的类脂质组成发生变化,在夏季样品中生物成因组分的比例明显高于冬季样品,此外随着纬度的增加,正烷烃的Cmax有增加的趋势,这一点主要反映了环境温度的变化。
其他摘要At present, international studies of atmospheric aerosols remains a lower level in the environmental organic geochemistry and it is still a blank in China. This dissertation is aimed at energy pollution problems demanding prompt solution related to coal, petroleum in our country. The lipid composition, source, and distribution in the atmosphere of aerosols from several cities in China were first systematically investigated by applying some concepts and indexes such as the distributions of homologous compounds, carbon preference index (CPI), and molecular markers etc. in organicygeochemistry and petroleum geochemistry. This dissertation described how to recognize atmospheric pollution produced from using and storing various kinds of fossil fuels. At the same time, it presented the distribution regularity of the pollutants in different region and climate band in China, and sampling heights, season effect atmospheric pollution. This will be very helpful for recognizing serious atmospheric pollution in China and effect factors. Twenty-eight aerosol samples are acquired from the suburb and urban sites in Beijing, Guangzhou, Guiyian and Shuicheng by filtration of ambient air using a standard air sampler. There are some samples eming from stationary sources such as coking factory, refining plants and tyre factory, and background region. All of collected sample filters are ultrasonically extracted in organic solvents. The extracts are esterified and then separated by TLC to yield the hydrocarbon, ester, aldehyde and ketone, and alcohol fractions. The alcohol fractions were converted to trimethylsilyl esters. Finally, compound molecular structure of the fractions were characterized by GC and GC/MS. Environmental organic geochemistry study of the analytical indicates: (1) There are close relationship between the different pollution sources and background site with the composition of atmospheric aerosols. The composition of lipids of aerosolsat stationary sources obviously reflect anthropogenic characterization and in background mainly demonstrate biogenic characteristcs. It is found that the burning products of coal (especially soft coal) contain numerous heterocyclic aromatic hydrocarbons and their oxygenated products, and waster gas of automobile and oil refining plant contain more triterpenoids. Complicated series of alkyl benzen compounds are found in the aerosol derect from petroleum products; (2) Normal alkanes, fatty acids, fatty alcohols, aromatic hydrocarbons, sesterdi- and triterpenoids, and steranes are commonly present in the atmospheric aerosols of four cities in China. These compounds derived from natural biogenic, geologic, synthetic sources, and are present in different proportion. The composition of lipids in the various city aerosols have much to do with their industry development, traffic and population density, and geographic conditions. Generally, the pollution level of suburbs atmosphere is much lower than that in urban; (3) The sampling height is a factor affecting the composition of lipids and the distribution of homologous of aerosols. Some apparent fractionation phenomena of lipid yields of aerosols are observed in samples from different heights above ground. (4) Season is also an important factor impact on the composition of aerosols. Samples in summer contain more biogenic lipids than that in winter.
页数142
语种中文
文献类型学位论文
条目标识符http://ir.gyig.ac.cn/handle/352002/3824
专题研究生_研究生_学位论文
推荐引用方式
GB/T 7714
张健. 中国几个城市低对流层大气颗粒中类脂质的特征及其环境有机地球化学意义[D]. 中国科学院地球化学研究所. 中国科学院地球化学研究所,1990.
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