中文题名: | 北京大气气溶胶、沙尘暴的理化特性及颗粒物的暴露评价研究 |
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保密级别: | 公开 |
学科代码: | 070304 |
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学生类型: | 博士 |
学位: | 理学博士 |
学位年度: | 2007 |
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研究方向: | 大气环境化学 |
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第一导师单位: | |
提交日期: | 2007-06-06 |
答辩日期: | 2007-06-02 |
外文题名: | PHYSICOCHEMICAL CHARACTERISTICS OF AIRBORNE PARTICULATE MATTER IN BEIJING AND RESEARCH ON BIOMARKERS OF POCYCLIC AROMATIC HYDROCARBONS |
中文关键词: | |
中文摘要: |
基于2000-2006七年的气溶胶外环境、2004-2005两年的气溶胶个体暴露和环境暴露人群生物指标的监测数据,综合ICP-AES、IC和HPLC等多种化学分析手段,采用富集系数、元素/离子特征比、图像分析、后项轨迹包括频数分析、相关性分析等在内的多种统计学分析方法,系统全面地研究了以北京为代表的中国典型地区大气颗粒物的环境污染特征及个体暴露水平及它们之间的相互影响,研究了环境暴露下特定人群如交通警察等的个体暴露PM2.5及其共存污染物水平,并寻找合适的生物标志物对污染物在人体内的内暴露水平进行分析。外环境气溶胶的污染研究包括颗粒物的年际变化、季节变化特征等长期变化规律及与气象条件和源排放特征之间相互关系的短期影响因素,分析了气溶胶的粒径分布、化学组成、来源、时空分布、转化机制及其与气象因素之间的相互影响。此外,还对中国北方沙尘暴尤其是2006年4月一次特大降尘进行了系统的监测和研究,并对两次不同类型的沙尘暴—强度弱但是污染性强的DS1(4月8-10日)和强度大但是沙尘特性强的DS2(4月16-18日),从其粒径分布、化学成分、组成来源特征、元素比值等多方面进行了分析,不同侧面均表明了DS1为“污染暴”,而DS2是典型的“沙尘暴”,并通过后向轨迹对于两次沙尘暴的差异给予了很好的解释,DS1由于在高、低空来源途径不一致,高空来自西部沙尘区而低空来自污染重的南部地区使其污染元素浓度增加较多,而DS2高、低空均来自西北和北部的沙尘区,属典型沙尘源区,地壳元素浓度较高。研究了细颗粒物PM2.5及其共存多环芳烃PAHs、挥发性有机污染物VOCs的人群个体暴露水平,并与相应的外环境水平进行比较,结果表明北京交通环境暴露下人群的个体暴露PM2.5污染较重,且受外环境浓度的影响变化较大,一般要高于相应的环境水平约20-30%,但不具有统计学差异,可以用环境浓度代替个体暴露水平,但是其共存PAHs的个体暴露水平要显著高于外环境水平,不能用外环境浓度来代替。PAHs中芘与BaP和总TPAH之间较好的相关性也表明了用芘的代谢产物尿中1-OHP作为PAHs生物标志物具有可行性,而结果也表明了这点。为更好的了解污染物的内暴露情况,选择合适的生物标志物针对环境暴露下特殊职业人群如交通警察、保安、交通协管员等进行研究,选择了尿中1-OHP和t,t-MA作为污染物PM2.5及其共存PAHs及挥发性有机污染物苯的低剂量暴露的接触生物标志物进行了分析,结果表明尿中1-OHP表现出了灵敏的生物标志物特性,而t,t-MA则未观察到较高的灵敏度,这可能是由于仪器检测限不够低和其他混杂因素如吸烟和食品添加剂等的影响,也为今后进一步寻找其它合适的苯系物标志物提供了有益的信息。
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外文摘要: |
The ambient level and personal exposure of atmospheric particulate matter, and the biomarkers of environmental exposure in Beijing, a typical metropolitan city of China were systematically studied. A seven-year long term aerosol samples from 2000 to 2006, a two-year personal exposure samples from 2004 to 2005 were collected, and then analyzed by ICP-AES, IC, and HPLC. The data were analyzed by combining enrichment factors, elemental/ionic/PAHs signatures, graphical techniques, back trajectory analysis, and multi-statistical analysis including spectral-density analysis and correlation analysis. A comprehensive study of particulate matter pollution, including particulate seasonal and short-term variation, size distributions, composition, and sources and its relation with meteorology and source emission were discussed in Beijing. In addition, the two dust storms in northern China in 2006 was systematically monitored and its composition, sources, and transformation were investigated. Two different kinds of dust storms were observed during the sampling time: weaker but polluted DS1 (8-10 April), and stronger and mineral DS2 (16-18 April). DS1 showed more pollution characteristics such as higher pollution elements and ions, higher pollutant elements’ EFs, and higher accumulations to fine particles but relatively lower concentration in coarse particles and crustal elements, and was named “pollution storm”. DS2 showed the contrary characteristics, i.e. the accumulation in coarse particles and higher crustal constitutes but lower pollution species and PAHs, and was named “dust storm”. The backward trajectory analysis gave the interesting explanation for the pollution of DS1, and mineral of DS2, i.e. the west direction in higher altitude for dust and south or southwest direction in lower altitude for pollution in DS1, the northwest and north transport pathways for DS2 in lower and higher altitude for pure dust in DS2. The personal exposure of PM2.5 and co-pollutants PAHs, and the volatile organic compounds were studied, and compared the personal exposure with relatively ambient level. Those who worked under ambient environments such as traffic policemen and safeguards outdoor were also selected to study the urine samples for biomarker analysis. Results showed that personal exposure of PM2.5 didn’t show statistically difference with the ambient level, which may be instituted by the ambient PM2.5 level. However, the personal exposure of PAHs showed significantly higher level than those ambient concentration, which may implied that the personal exposure of PAHs could not be instituted by the ambient level. Both the ambient concentration and the personal exposure of pyrene, BaP, and the total TPAH in PM2.5 showed good correlations, suggesting the great value of 1-OHP, the major urinary metabolite of pyrene, to be the biomarker of BaP and TPAH. As the major metabolites of atmospheric pyrene and benzene in urine, the urinary 1-hydroxypyrene (1-OHP) and trans, trans-muconic acid (t,t-MA) were selected to be the biomarker of them. Results showed that 1-OHP is a relatively coarse biomarker, and did not respond sensitively enough to the scale of differences in personal exposures to PAHs between the exposed and control group (30% or so), which implies that future studies need to build in bigger differences in exposures. Furthermore, smoking provided as much exposure to PAHs as the ambient aerosol did, and so represented a major confounding factor, and need to be controlled very carefully in the future. Urinary t,t-MA seems not so sensitively enough to be the biomarker of benzene, as smoke and the food additives sorbic acid, the limitation of instrumental analysis may impacts the urinary t,t-MA detection. This may imply that the better biomarkers of benzene, s-phenylmercapturic acid need to be studied more in the future.
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参考文献总数: | 89 |
作者简介: | 张文杰,本科以优秀成绩从山东考入本校研究生。自进入研究生学习以来,各门成绩优秀, 逐步显露出较强的创造性思维、严谨的科学态度和优秀的科研能力。 她参加了大气环境研究中心各个重大重点项目研究达五年之久,并于2004年3月开始在中国疾病预防控制中心环境所参加空气质量监测室的各项重大项目,参加了大气化学分析实验室的建设,参与建立了包括我国从西北内陆多伦、榆林,经由北京、青岛、上海到内海的多个同步监测采样站点,累积了大量的实地监测分析数据。熟练掌握从事环境相关专业所必需的采样和现代仪器分析技术(IC、ICP、GCMS、HPLC、LC等),具有很强的动手实验能力和创新能力,成功建立了高效液相分析气溶胶中多环芳烃、尿中1-羟基芘和粘糠酸的方法,已成为气溶胶分析和尿样分析的常用的方法,对我国气溶胶科学有关的研究起了很大作用。她采用环境化学、化学统计学与分子生物学等多种方法相结合,从对大气污染物的环境监测到个体暴露直至内暴露生物标志物的分析,通过外环境-个体外暴露-内暴露生物标志物三者互相结合研究,对于推动学科交叉发展起到重要作用。 张文杰能够熟练运用英语读、听、写、说,能流利地与国外同行交流沟通,能独立撰写科学论文。现已经有多篇论文发表在国内外杂志上,其中有SCI文章英文4篇,SCIE和ISTP各1篇,还有一篇正在被审阅。博士论文“北京大气气溶胶、沙尘暴的理化特性及颗粒物的暴露评价研究”选题明确,创新性很高,从气溶胶外环境水平、个体暴露水平和人体内暴露生物标志物三个方面,层层深入的研究了北京气溶胶的地区性污染状况,对环境暴露下人群如交通警察等的个体暴露水平进行了研究,并同时研究了其生物标志物的内暴露水平,为国家环境保护有关部门提供了第一手的宝贵资料。不仅对国际大气科学尤其是气溶胶科学有相当理论意义,而且对全球环境变化和中国的主要环境问题(如城市空气污染问题)有重大应用价值,是当前国际上大气科学研究的前沿。 |
馆藏地: | 图书馆学位论文阅览区(主馆南区三层BC区) |
馆藏号: | 博070304/0711 |
开放日期: | 2007-06-06 |