生物质燃烧烟雾和大气降尘中多环芳烃及其烷基取代物的研究
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摘要
多环芳烃及其烷基取代物是一类具有强致畸致癌性的持久性有机污染物,主要来源于有机物的燃烧。除了石油和煤等化石燃料产生多环芳烃外,生物质的燃烧也是其重要来源。我国的生物质资源丰富,每年有6亿吨的农作物秸秆产生。其中,31.5%用作农村地区的炊事能源,25%在农田中就地焚烧。生物质燃烧排放出多种污染物,引起了较多的关注。但目前,我国在生物质燃烧排放多环芳烃类污染物方面的研究很少。针对这种状况,本文设计了秸秆燃烧和采样系统,采集秸秆燃烧后释放的多环芳烃及其烷基取代物,分析其种类、浓度和气相—颗粒相分布,并对影响多环芳烃排放的因素和排放特征进行了探讨.根据实验数据,计算了三种秸秆燃烧产生的多环芳烃的排放因子和我国每年秸秆燃烧产生的多环芳烃的总量以及毒性当量。
2003年上海市环境空气质量报告指出,降尘污染负荷系数居全市主要污染物之首。而降尘作为大气中其他颗粒物的重要的源和汇的之一,但目前对降尘及其中的有机污染物的研究很少。本论文对上海降尘中烷基多环芳烃的组成、时空分布、来源和环境影响进行了详细的分析和探讨.
本论文主要包括三个部分。
第一部分为分析方法的优化。本文采用超临界流体萃取技术作为样品的萃取手段。先用模拟样品对影响APAHs萃取的实验条件进行探讨,然后用正交法对实际样品进行分析,以优化萃取条件。
第二部分应用上述建立的分析方法检测了从2004年11月到2005年11月分季节上海市不同功能区的13个采样点的降尘样品中的APAHs的组成、浓度,并与PAHs进行了对比。同时,对其时空分布特点、源解析和对环境的影响做了研究。
第三部分为秸秆燃烧排放多环芳烃及其烷基取代物的研究。针对我国生物质燃烧的现状,设计了模拟燃烧和采样的装置,采集并分析了三种我国主要的秸秆燃烧排放的TSP和多环芳烃及其烷基取代物。对不同秸秆燃烧排放的多环芳烃类化合物的组成、浓度和气相—颗粒相分布进行了分析。同时,对影响秸秆燃烧排放多环芳烃的因素进行了探讨。
在此基础上,得到了不同秸秆燃烧排放的多环芳烃的排放因子,并计算了我国每年通过秸秆燃烧排放的TSP和多环芳烃的总量及其毒性当量。同时,还应用比值法和主成分因子分析法对秸秆燃烧源的多环芳烃的排放特征进行了研究。
Polycyclic aromatic hydrocarbons (PAHs) and their alkyl derivatives (APAHs) are a group of persistent organic pollutants (POPs) which largely resulted from combustion of fuels including oil, coal and biomass. There is a large amount of biomass in China, where 600 millions tons of straw are harvested every year. 31.5% of them were used as the residential energy source for cooking, and 25% were burnt in the field for land-clearing. Many pollutants were emitted form biomass burning, and more attentions were paid in the worldwide. However, little work was done on this field in China. So, a set of apparatus was designed and installed to simulate biomass burning. Total suspended particulate and PAHs/APAHs were sampled and analyzed to get emission factors (EF) of PAHs and APAHs and the total flux of PAHs/APAHs emitted from biomass burning.
Dustfall is one of the main atmospheric components in the urbanized area. With the fast development of population and motors during the last decades, the atmospheric particulate matter has become one of the main issues in Shanghai. And in the Reports of Environmental Quality of Shanghai in 2003, dustfall is identified as the most abundant pollutant in urban, suburban and rural areas. By now, the research on the organic pollutants in dustfall in this megacity remains scarce. The objective of the present work was to determine the profiles, levels and spatial-temporal distribution of APAHs in dust, distinguish the sources and estimate the effect on the coastal environment.
This work consists of three main parts, as following:
The first part introduces the parameters optimization of supercritical fluid extraction. Simulative samples were employed for the selection of parameters, and real-world samples were extracted by orthotropic experiments to optimize the extraction conditions.
In the second part, dustfall samples were collected form 13 sites in urban area of Shanghai from Nov, 2004 to Nov, 2005, and analyze by the above method. Profiles and levels of APAHs were obtained and compared with PAHs. On this basis, spatial-temporal distribution, sources and effect on environment were investigated.
In the last part, PAHs/APAHs emitted from biomass burning were researched in detail. A set of apparatus was designed and installed to simulate biomass burning. TSP and PAHs/APAHs were collected from the smog of three straws burning, and analyzed for species, levels and the gas-particle partitioning. Further more, factors controlled PAHs/APAHs emission from biomass burning were explained. According to experimental data, emission factors (EF) of PAHs and APAHs were calculated, and then the total flux of PAHs/APAHs emtted from biomass burning was estimated.
2003年上海市环境空气质量报告指出,降尘污染负荷系数居全市主要污染物之首。而降尘作为大气中其他颗粒物的重要的源和汇的之一,但目前对降尘及其中的有机污染物的研究很少。本论文对上海降尘中烷基多环芳烃的组成、时空分布、来源和环境影响进行了详细的分析和探讨.
本论文主要包括三个部分。
第一部分为分析方法的优化。本文采用超临界流体萃取技术作为样品的萃取手段。先用模拟样品对影响APAHs萃取的实验条件进行探讨,然后用正交法对实际样品进行分析,以优化萃取条件。
第二部分应用上述建立的分析方法检测了从2004年11月到2005年11月分季节上海市不同功能区的13个采样点的降尘样品中的APAHs的组成、浓度,并与PAHs进行了对比。同时,对其时空分布特点、源解析和对环境的影响做了研究。
第三部分为秸秆燃烧排放多环芳烃及其烷基取代物的研究。针对我国生物质燃烧的现状,设计了模拟燃烧和采样的装置,采集并分析了三种我国主要的秸秆燃烧排放的TSP和多环芳烃及其烷基取代物。对不同秸秆燃烧排放的多环芳烃类化合物的组成、浓度和气相—颗粒相分布进行了分析。同时,对影响秸秆燃烧排放多环芳烃的因素进行了探讨。
在此基础上,得到了不同秸秆燃烧排放的多环芳烃的排放因子,并计算了我国每年通过秸秆燃烧排放的TSP和多环芳烃的总量及其毒性当量。同时,还应用比值法和主成分因子分析法对秸秆燃烧源的多环芳烃的排放特征进行了研究。
Polycyclic aromatic hydrocarbons (PAHs) and their alkyl derivatives (APAHs) are a group of persistent organic pollutants (POPs) which largely resulted from combustion of fuels including oil, coal and biomass. There is a large amount of biomass in China, where 600 millions tons of straw are harvested every year. 31.5% of them were used as the residential energy source for cooking, and 25% were burnt in the field for land-clearing. Many pollutants were emitted form biomass burning, and more attentions were paid in the worldwide. However, little work was done on this field in China. So, a set of apparatus was designed and installed to simulate biomass burning. Total suspended particulate and PAHs/APAHs were sampled and analyzed to get emission factors (EF) of PAHs and APAHs and the total flux of PAHs/APAHs emitted from biomass burning.
Dustfall is one of the main atmospheric components in the urbanized area. With the fast development of population and motors during the last decades, the atmospheric particulate matter has become one of the main issues in Shanghai. And in the Reports of Environmental Quality of Shanghai in 2003, dustfall is identified as the most abundant pollutant in urban, suburban and rural areas. By now, the research on the organic pollutants in dustfall in this megacity remains scarce. The objective of the present work was to determine the profiles, levels and spatial-temporal distribution of APAHs in dust, distinguish the sources and estimate the effect on the coastal environment.
This work consists of three main parts, as following:
The first part introduces the parameters optimization of supercritical fluid extraction. Simulative samples were employed for the selection of parameters, and real-world samples were extracted by orthotropic experiments to optimize the extraction conditions.
In the second part, dustfall samples were collected form 13 sites in urban area of Shanghai from Nov, 2004 to Nov, 2005, and analyze by the above method. Profiles and levels of APAHs were obtained and compared with PAHs. On this basis, spatial-temporal distribution, sources and effect on environment were investigated.
In the last part, PAHs/APAHs emitted from biomass burning were researched in detail. A set of apparatus was designed and installed to simulate biomass burning. TSP and PAHs/APAHs were collected from the smog of three straws burning, and analyzed for species, levels and the gas-particle partitioning. Further more, factors controlled PAHs/APAHs emission from biomass burning were explained. According to experimental data, emission factors (EF) of PAHs and APAHs were calculated, and then the total flux of PAHs/APAHs emtted from biomass burning was estimated.
引文
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