住宅室内降尘中多环芳烃污染研究与预警系统构建

发布时间：2018-01-06 12:34

本文关键词：住宅室内降尘中多环芳烃污染研究与预警系统构建　出处：《重庆大学》2015年博士论文　论文类型：学位论文

【摘要】：多环芳烃(Polycyclic aromatic hydrocarbons,简称PAHs),是一类典型持久性有机污染物,是环境中的重要致癌物质之一。PAHs对环境的污染无处不在,人类已经在大气、水体、土壤、农作物、食品等样品中检测到了不同种类的PAHs污染物。PAHs污染具有“三大特性”,即:明显毒性(致癌、致畸、致突变)、长期残留性和生物蓄积性,因此,PAHs的研究受到了国内外政府组织与专家学者的广泛关注。降尘是指在自身重力作用下可以沉降到地面上的颗粒物,它对生态系统的破坏具有隐蔽性、潜在性和长期性。室内降尘作为多种污染物的载体,能直接或间接被人体吸入或摄入,诱发多种疾病。随着社会经济的不断发展,人们对环境污染的关注度越来越高,由于人类超过80%的时间暴露于室内,室内环境污染方面的研究正日益受到重视,室内降尘污染研究也不例外。但是,迄今为止,国内外关于室内降尘中PAHs污染方面的研究较少,我国西部地区由于经济发展水平相对落后,对室内降尘中PAHs污染研究就更少,甚至处于空白状态。自国家确立“西部大开发”战略以来,西部地区的社会经济得到了极大的发展和提升,但随之而来的环境污染问题也日益突出。寻找合适的研究载体为突破口,掌握环境污染的第一手资料和信息,探讨其分布规律与影响因素,构建科学合理的污染预警系统,对协调我国西部地区发展经济与环境保护之间的关系,促进地方经济以环境友好为前提的可持续发展和再快速提升发展具有重要意义。因此,本文针对我国西部地区室内降尘中PAHs研究匮乏的现状,以西部代表性区域贵州省为研究示范,开展了室内降尘中PAHs的污染现状、季节变化、区域分布规律、风险特征等研究,并在此基础上构建了基于指纹识别理论的PAHs预警系统,为西部地区室内环境保护提供理论依据和技术支撑。主要内容如下:第一部分,室内降尘PAHs污染预警系统构建方法和理论研究。PAHs污染组成复杂,种类繁多,且目前缺乏能同时对上百种PAHs污染进行监控和预警的方法。为此,本文借鉴指纹识别理论,结合现代色谱分析技术和模式识别统计方法,构建基于指纹图谱技术的PAHs污染预警系统的理论框架,以实现对上百种PAHs污染物的整体监控。第二部分,室内降尘中代表性PAHs污染物现状及分布规律研究。为实现预警系统的构建,优先对当前国际上要求严控的18种PAHs进行研究,摸清其污染现状,分析其分布规律,探讨其影响因素,为预警系统的构建提供重要依据。主要工作如下:首先,完成了18种pahs的高效液相色谱定量分析方法构建。18种pahs污染物在0.2-2.0μg范围内线性关系良好,相关系数γ均大于0.9992,检出限和定量限分别为6.18-12.58ng和20.6-41.93ng;各pahs组分的平均回收率在91.61%-102.81%之间,相对平均标准偏差rsd值为1.06%-3.24%。同时,利用所建立的pahs定量分析方法,对2012-2013年采集的贵州省全部9个地级行政区(涉及13个市县、22个乡镇和52个村)的住宅室内降尘样品进行测试分析。结果显示,贵州室内降尘中的Σ18pahs平均含量为1.61μg·g-1,不同行政区Σ18pahs含量有较大差异;整个研究区域pahs污染物种类以高环(4-6环)pahs为主,尤以phe、flt和pyr为最优势物种。在室内降尘中18种pahs污染物特征及现状分析基础上,进一步对pahs污染的季节变化和区域分布特征进行研究,为后续建立pahs污染预警系统提供基础数据。研究结果表明:冬季Σ18pahs水平比夏季高,大量燃用煤和生物质的季节性排放是导致室内降尘Σ18pahs冬夏浓度出现差异的主要因素;Σ18pahs的行政区域分布与人口密度的线性相关系数为0.91,显示出人为活动带来的排放是室内降尘pahs分布的重要驱动因子。Σ18pahs含量存在显著的城乡趋势,市县Σ18pahs平均浓度分别是乡镇和农村的1.6倍和2.7倍,但农村地区面临发展经济和保护环境的双重压力比城镇更为严峻。最优尺度回归模型表明:行政区、城乡区域、季节、采样楼层、距主干道距离均是影响室内降尘Σ18pahs浓度水平的重要因素,且行政区和城乡区域对室内降尘Σ18pahs浓度的影响最大。第三部分,pahs污染的来源解析及暴露风险评价。源解析和暴露风险评价是pahs污染研究的重要组成部分,研究成果可为环境污染相关标准的制订提供理论基础,也为pahs污染预警系统的构建提供重要依据。本文采用特征化合物法和主成分分析/多元线性回归法对室内降尘中Σ18pahs的来源进行解析,结果表明:室内降尘Σ18pahs浓度受室外和室内环境因素的共同影响,其中交通排放和燃煤排放对室内降尘Σ18pahs的影响较大;市县住宅燃煤排放源主要来自室外,而农村住宅室内环境中存在直接的煤炭燃烧源,直接向室内环境释放一定含量的pahs。对住宅室内降尘Σ18pahs的健康风险评价结果表明:对皮肤接触和吞食降尘而引起的终生致癌风险(ilcrs),儿童和成人的平均ilcrs均超过了10-7,远大于因呼吸摄入引起的致癌风险(平均ilcrs小于10-10)。总的来说,儿童对室内降尘pahs引发的总致癌风险率要高于成人,且蒙特卡罗不确定性分析结果表明,儿童对室内降尘Σ18pahs污染物的暴露时间更为敏感。第四部分,室内降尘pahs污染预警系统构建及运行示范。在前述室内降尘pahs污染预警系统构建方法和理论研究基础上,结合对18种代表性pahs污染物研究获得的基础性数据与结论,以贵州省为示范地点,将所建立的pahs预警理论和方法进行了实践应用。建立了室内降尘中PAHs指纹图谱采集方法;构建了贵州地区特征图谱库,获得了市县、乡镇和农村住宅室内降尘PAHs污染特征图谱27幅;成功构建了贵州地区基于指纹识别技术的室内降尘PAHs污染预警系统,该预警系统由指纹图谱采集、特征图谱提取、特征图谱库、图谱匹配处理以及结果输出等核心模块组成。并以贵阳地区为例,对所建立的PAHs污染预警系统进行运行示范研究,通过采集实时样品,分析贵阳地区室内降尘中PAHs的实时污染状况,预测了其污染趋势,验证了本文所建立的预警系统能够实现对室内降尘中上百种PAHs的整体监控和预警。
[Abstract]:Polycyclic aromatic hydrocarbons (Polycyclic aromatic hydrocarbons, referred to as PAHs), is a kind of typical persistent organic pollutants, is an important one of the carcinogens in the environment of.PAHs pollution everywhere on the environment, human beings have in the atmosphere, water, soil, crops and food samples were detected in different types of PAHs.PAHs with "three pollution pollutants namely: characteristics, toxicity (carcinogenic, teratogenic, mutagenic), environmental persistence, bioaccumulation, therefore, the research of PAHs has attracted extensive attention of the government organization and domestic experts and scholars. The dust is under its own gravity can settle to particles on the ground, its damage to the ecological the system has a hidden, potential and long-term indoor dust. As a carrier of various pollutants, which can directly or indirectly be inhaled or ingested, cause a variety of diseases. With the continuous development of social economy, The environmental pollution has been paid more and more attention, because more than 80% of human exposure to indoor environmental pollution, indoor research is more and more attention, research on reducing indoor dust pollution is no exception. However, so far, the domestic and foreign research on indoor PAHs pollution in reducing dust less, because the level of economic development the relatively backward western region of our country, dust pollution of PAHs is less on the interior, even in a blank state. Since the establishment of the "western development" strategy, the western region's social economy has been greatly developed and improved, but the attendant environmental problems have become increasingly prominent. Research on finding suitable vector as a breakthrough environmental pollution, master first-hand data and information, the distribution regularity and influence factors, construction of pollution warning system is scientific and reasonable coordination of western region development in China The relationship between the economy and environmental protection, promote the sustainable development of the local economy in the premise of environmental friendly and has important significance to enhance the rapid development. Therefore, according to the interior in the western area of China reduced the current status of the dust in PAHs research is scarce, in the western representative areas of Guizhou Province as the research model, the pollution situation, carry out indoor drop the dust PAHs seasonal changes, regional distribution of risk characteristics, and on the basis of constructing the PAHs warning system based on fingerprint identification theory, provide theoretical basis and technical support for the protection of the indoor environment in the western region. The main contents are as follows: the first part, the indoor dust pollution warning system PAHs construction method and theory research.PAHs the pollution of complex composition, variety, and the current lack of methods for simultaneous monitoring and early warning of hundreds of PAHs pollution. Therefore, based on fingerprint recognition theory, Combined with the analysis of technology and statistical pattern recognition method of modern chromatography, constructs the theoretical framework of PAHs pollution warning system based on fingerprint technology, based on hundreds of PAHs pollutants overall monitoring. The second part of the status and distribution of PAHs indoor pollutants reduction law research on behalf of dust. For construction of early warning system, research the priority of 18 PAHs on the current international strict control, to find out the pollution situation, analyze the distribution, to explore its influencing factors, provide an important basis for the construction of the early warning system. The main work is as follows: first, finished 18 PAHs quantitative high performance liquid chromatography analysis method to construct the.18 PAHs pollutants in 0.2-2.0 g good linear range, correlation coefficient r was greater than 0.9992, and quantification limit of detection were 6.18-12.58ng and 20.6-41.93ng; the PAHs component of the average recovery rate was 91.61% -102.81% The relative standard deviation, average RSD value of 1.06%-3.24%. at the same time, by using the PAHs analysis method based on quantitative, 2012-2013 years collected in Guizhou province all 9 prefecture level administrative region (involving 13 counties, 22 towns and 52 villages) were tested and analyzed the indoor dust samples. The results showed that the average content of sigma 18pahs in Dustfall of Guizhou chamber of 1.61 G - g-1, there is great difference in different administrative region 18pahs content; the entire study area of PAHs pollutants with high ring (4-6 rings) PAHs, especially Phe, FLT and Pyr were the most dominant species. In the indoor 18 characteristics and the current situation of PAHs pollutants analysis in the dust, the further research of PAHs pollution seasonal changes and regional distribution, to provide the basic data for the subsequent establishment of PAHs pollution warning system. The results show that: Sigma 18pahs level was higher than that in summer winter, seasonal discharge burning a lot of coal and biomass Let is the cause of dust concentration in winter 18pahs sigma factors difference; linear correlation coefficient of the administrative area of distribution and population density of sigma 18pahs was 0.91, showing human activities bring dust emission is an important driving factor of PAHs distribution. There is a significant trend in urban and rural areas the total 18pahs content, and the average concentration of 18pahs sigma are 1.6 times and 2.7 times of the towns and rural areas, but rural areas face the dual pressures of economic development and protect the environment than in cities is more severe. The optimal scale regression model showed that the administrative region, urban and rural areas, seasons, sampling floors, the main road distance is an important factor affecting the dust concentration level of 18pahs the influence and the administrative region and urban and rural areas of dust total 18pahs concentration maximum. In the third part, the source apportionment of PAHs pollution and risk assessment. Source apportionment and exposure risk assessment is PAHs. An important part of the dye, provide theoretical basis for the research results of environmental pollution related standards, but also provide an important basis for the construction of PAHs pollution warning system. This paper uses the analysis / characteristic compound method and principal component analysis, the source of dust on the indoor 18pahs multivariate linear regression method. The results showed that the influence of dust total 18pahs concentration by outdoor and indoor environmental factors, which affect the traffic emissions and emissions of coal dust 18pahs; and residential coal emissions are mainly sourced from the outside, while the rural living existence of coal combustion source directly home indoor environment, health risk assessment of the release of certain content directly to the indoor environment pahs. of residential indoor dust Sigma 18pahs results indicated that the skin contact and ingestion of dust caused by cancer risk (ilcrs), the average ilcrs of children and adults are More than 10-7, far greater than the intake of carcinogenic risk caused by breathing (average ilcrs less than 10-10). In general, children of dust caused by PAHs the total cancer risk rate is higher than that of adults, and Monte Carlo uncertainty analysis results show that the exposure time of children's indoor dust pollution is more sensitive to 18pahs fourth. Part of indoor construction dust reduction PAHs pollution early warning system and operation demonstration. In the indoor drop foundation method and theoretical research on the construction of PAHs dust pollution warning system, combined with the basic number of research on 18 typical PAHs pollutants and according to the conclusion, taking Guizhou Province as demonstration sites, the PAHs early warning theory and method of application. Established PAHs fingerprint collecting dust reduction method for indoor; construction of Guizhou area characteristic map database, obtained the counties, towns and rural residential indoor dust pollution characteristics of PAHs 27 patterns; the successful construction of the Guizhou area of fingerprint recognition technology based on PAHs indoor dust pollution warning system, the warning system consists of fingerprint acquisition, fingerprint feature extraction, map database, map matching processing and result output module. The core and takes Guiyang as an example, to run the demonstration research on PAHs pollution warning this system, by collecting samples in real time, real-time analysis of pollution condition of Guiyang area dust in PAHs, predicts the trend of the pollution, the overall monitoring and early warning warning system to verify the proposed in this paper can realize the reduction of hundreds of PAHs dust on the indoor.

【学位授予单位】：重庆大学
【学位级别】：博士
【学位授予年份】：2015
【分类号】：X51;TU834.6

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