关中地区PM2.5的时空分布特征及来源解析-硕士论文.docx

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1、密级: 硕士学位论文关中地区 PM2.5 的时空分布特征及来源解析作者姓名: 指导教师: 学位类别: 理学硕士 学科专业: 环境科学 研究所: 年 月Error! No text of specified style in document.I致谢三年的时光如白驹过隙,转瞬即逝。仍记得 2012 年春季刚到所里时与研究员交流的情景,韩老师的和蔼和曹老师的爽朗给我留下了深刻的印象。硕士生面试通过后,我正式成为了粉尘与环境研究室的一员,成为了韩老师的学生。在研究生期间,韩老师对待科研求真务实的态度和孜孜不倦的精神令我十分敬佩,让我对科研及人生道路都有了新的认识和领悟;同时,韩老师在工作和学习上也常

2、会给予我点播和指导,在生活上也常会给予我关怀和帮助,使我少走弯路,迅速成长。曹老师作为研究室领军人物,为我们提供了优秀的科研平台,创建了浓厚的科研氛围,身处其中,我也受益匪浅;同时,曹老师热情开朗的性格和饱满昂扬的斗志,让我也学会了在面对困难时不屈不挠,顽强克服的品质。值此论文完成之际,谨向我的导师韩老师和曹老师致以最诚挚的感谢和最崇高的敬意。最后也是最重要的,感谢我的家人二十多年来对我的关心、鼓励、理解和支持,我爱你们。关中地区 PM2.5 的时空分布特征及来源解析II关中地区 PM2.5 的时空分布特征及来源解析摘要为探讨关中地区 PM2.5 的污染特征及来源构成,本研究于 2012 年

3、3 月至2013 年 2 月在西安、宝鸡、渭南和秦岭进行了 PM2.5 的采集,分析了其质量浓度、元素、水溶性无机离子和碳组分的时空变化特征,并利用 PMF 和 CMB 模型分析了各排放源对关中地区 PM2.5 的贡献。主要结论如下:采样期间,西安、宝鸡、渭南和秦岭 PM2.5 的年均浓度分别为(156.1102.8)gm-3、(118.477.7)gm -3、(123.669.7)gm -3 和(109.382.9)gm -3。PM 2.5 的季节变化表现为:冬季最高,夏季最低,春季和秋季居中。空间变化上,春季时西安宝鸡渭南秦岭,夏季时西安渭南宝鸡秦岭,秋季时西安渭南秦岭宝鸡,冬季时西安秦岭

4、宝鸡渭南。元素、水溶性无机离子和碳组分同样表现出一定的空间和时间变化。其中,Al、Si、Ca 、Fe 和 Zn 是各采样点的主要元素,Al、Si、Ca、Ti 和 Fe 主要来自于自然源,Cr 和 Mn 同时受到自然源和人为源的共同影响,Zn、As、Br 和 Pb 主要来自于人为源。二次水溶性无机离子 SO42-、NO 3-和 NH4+是含量最高的离子,三者之和约占总离子的 80%90%。各采样点 SO42-、NO 3-和 NH4+的浓度均在冬季时最高,SO 42-在夏季的浓度也很高,仅次于冬季。NO 3-/SO42-的年均比值约为 0.730.76,表明关中地区的污染是以燃煤为代表的固定源为主

5、。各采样点 OC 浓度均在冬季最高,EC 浓度在各季节差别相对较小。空间变化上,西安在各季节的 OC 和 EC浓度均最高,尤其是冬季,这与 PM2.5 的浓度分布呈现出相同规律。物质平衡分析表明,关中地区全年 PM2.5 中 OM 所占比例最高,占22.7%31.7%,此外 SO42-、NO 3-和 GM 所占比例也较高,分别占15.2%21.0%、11.3%15.3%和 10.1%17.2%。从季节变化来看,春季时 GM和 OM 所占比例较高,分别占 18.7%28.4%和 17.9%28.6%;夏季时,SO 42-所占比例最高,占 24.0%36.1%,此外 OM 所占比例也较高,占 14

6、.5%21.1%;秋季时,OM 所占比例最高,占 26.2%34.8%;冬季时,OM 所占比例仍为最高,占 22.9%36.4%。Error! No text of specified style in document.IIIPMF 解析结果显示,二次硝酸盐、二次硫酸盐、燃煤、机动车、生物质燃烧和地质尘对西安全年 PM2.5 的贡献分别为15.2%、 20.1%、19.2%、 12.7%、12.8%和 13.1%,对宝鸡的贡献分别为15.1%、 22.9%、17.9%、 10.4%、15.4%和 12.6%,对渭南的贡献分别为14.7%、 22.7%、18.6%、 10.8%、14.8%和

7、12.2%,对秦岭的贡献分别为18.4%、 27.2%、10.9%、 9.8%、10.3%和 20.0%。CMB 源解析结果显示,二次硝酸盐、二次硫酸盐、燃煤、机动车、生物质燃烧和地质尘对西安全年 PM2.5的贡献分别为 13.3%、16.1%、22.9%、9.8% 、14.9% 和 15.8%,对宝鸡的贡献分别为 12.3%、 17.8%、21.0% 、8.6% 、16.2%和 16.0%,对渭南的贡献分别为11.9%、 15.8%、21.3%、 8.4%、15.7%和 15.1%,对秦岭的贡献分别为13.5%、 18.5%、14.4%、 7.5%、15.1%和 18.1%。春季时地质尘是各

8、采样点PM2.5 的首要来源,夏季时二次硫酸盐为首要来源,秋季时生物质的贡献较大,冬季时燃煤和二次硫酸盐贡献最大。在地质尘源中,城市地区的建筑尘贡献最大,秦岭的土壤尘贡献最大;在燃煤源中,工业燃煤的贡献大于家庭燃煤,但冬季时差距变小。关键词:PM 2.5,关中地区,时空分布,来源解析关中地区 PM2.5 的时空分布特征及来源解析IVSpatial and temporal distribution and source apportionment of PM2.5 in Guanzhong areaAbstractTo recognize the pollution characteristi

9、cs and sources of PM2.5 in Guanzhong, PM2.5 were sampled in Xian, Baoji, Weinan and Qinling from March 2012 to February 2013, and then PM2.5 mass, elements, water soluble inorganic ions and carbon compositions were analyzed. Finally, PMF and CMB were used to analyze the contribution of different sou

10、rces to PM2.5. The main results are as follows:During the sampling period, the annual concentrations of PM2.5 in Xian, Baoji, Weinan and Qinling were (156.1102.8) gm-3, (118.477.7) gm-3, (123.669.7) gm-3 and (109.382.9) gm-3, respectively. As to the seasonal variations, the highest concentration app

11、eared in winter, lowest in summer, and medial in spring and autumn. In the view of spatial variations, Xian Baoji Weinan Qinling in spring, Xian Weinan Baoji Qinling in summer, Xian Weinan Qinling Baoji in autumn, and Xian Qinling Baoji Weinan in winter. Elements, water soluble inorganic ions and ca

12、rbon compositions also showed spatial and temporal vatiations. Among the compositions, Al, Si, Ca, Fe and Zn were the major elements. The analysis of enrichment factor showed that Al, Si, Ca and Ti were mainly from natural sources, Cr and Mn were affected by natural and anthropogenic sources togethe

13、r, and Zn, As Br and Pb were mainly from anthropogenic sources. SO42-, NO3- and NH4+ were the major ions, and they accounted for 80%90% of the total ions. The concentration of SO42-, NO3- and NH4+ were highest in winter, and SO42- also had high concentration in summer. The annual ratios of NO3-/SO42

14、- were 0.730.76, which indicated that pollutants mainly came from stationary sources, especially coal combustion. OC showed the highest concentration in winter in all sites, however EC Error! No text of specified style in document.Vhad little differences among seasons. As to the spatial variation, X

15、ian had the highest OC and EC in all seasons, especially in winter, which showed the same variation with PM2.5.The analysis of material balance showed that OM, which accounted for 22.7%31.7% of PM2.5, was the main component of PM2.5 in Guanzhong. In addition, SO42-、 NO3- and GM also had high ratios,

16、 and they accounted for 5.2%21.0%, 11.3%15.3% and 10.1%17.2%, respectively. As to the seasonal variation, GM and OM, which accounted for 18.7%28.4% and 17.9%28.6%, respectively, were the main components in spring; SO42- and OM, which accounted for 24.0%36.1% and 14.5%21.1%, respectively, were the ma

17、in components in summer; OM, which accounted for 26.2%34.8% and 22.9%36.4%, respectively, were the main components in autumn and winter.The PMF results showed that the contribution of secondary nitrate, secondary sulfate, coal combustion, vehicle exhausts, biomass burning and geological material to

18、the annual PM2.5 were 15.2%, 20.1%, 19.2%, 12.7%, 12.8% and 13.1%, respectively in Xian; 15.1%, 22.9%, 17.9%, 10.4%, 15.4% and 12.6%, respectively in Baoji; 14.7%, 22.7%, 18.6%, 10.8%, 14.8% and 12.2%, respectively in Weinan; 18.4%, 27.2%, 10.9%, 9.8%, 10.3% and 20.0%, respectively in Qinling. The C

19、MB results showed that the contribution of secondary nitrate, secondary sulfate, coal combustion, vehicle exhausts, biomass burning and geological material to the annual PM2.5 were 13.3%, 16.1%, 22.9%, 9.8%, 14.9% and 15.8%, respectively in Xian; 12.3%, 17.8%, 21.0%, 8.6%, 16.2% and 16.0%, respectiv

20、ely in Baoji; 11.9%, 15.8%, 21.3%, 8.4%, 15.7% and 15.1%, respectively in Weinan; 13.5%, 18.5%, 14.4%, 7.5%, 15.1% and 18.1%, respectively in Qinling. In spring, geological material was the primary source; in summer, secondary sulfate was the primary source; in autumn, the contribution of biomass bu

21、rning was important; in winter, biomass burning and secondary sulfate were equal important. As to geological material, construction dust was the most important source in cities, especially in Xian, however soil dust was the most important source in Qinling. For the coal combustion, the contribution

22、of industry coal was larger than domestic coal, but smaller gap in winter.关中地区 PM2.5 的时空分布特征及来源解析VIKey words: PM2.5, Guanzhong area, spatial and temporal distribution, source apportionment目录i目录致 谢 .I摘 要 .IIIAbstract .V第一章 绪论 .11.1 PM2.5 简介 .11.1.1 PM2.5 的基本特征 .11.1.2 PM2.5 的主要来源 .41.2 研究意义 .51.3 研究现

23、状 .61.4 论文选题意义和研究内容 .71.4.1 论文选题意义 .71.4.2 论文研究内容 .71.4.3 研究路线 .81.4.4 论文创新点 .81.4.5 论文工作量 .9第二章 样品的采集与分析 .112.1 关中地区概况 .112.2 采样点布设及样品采集 .122.2.1 采样点布设 .122.2.2 样品采集 .132.3 样品分析 .132.3.1 PM2.5 质量浓度分析 .132.3.2 元素分析 .142.3.3 水溶性无机离子分析 .152.3.4 碳组分分析 .16第三章 PM2.5 及其化学组分的时空分布特征 .193.1 PM2.5 质量浓度变化特征 .1

24、93.1.1 全年变化特征 .19关中地区 PM2.5 的时空分布特征及来源解析ii3.1.2 季节变化特征 .203.1.3 月变化特征 .213.2 元素变化特征 .223.2.1 元素浓度变化特征 .223.2.2 富集因子分析 .233.2.3 地壳物质分析 .253.3 水溶性无机离子变化特征 .263.3.2 离子平衡分析 .283.3.3 离子相关性及结合方式 .293.4 碳组分变化特征 .303.4.1 OC/EC 浓度及比值变化特征 .303.4.2 OC/EC 相关性分析 .313.4.3 SOC 浓度分析 .323.5 发散系数 .33第四章 PM2.5 的物质平衡及来源解析 .374.1 PM2.5 的物质平衡 .374.2 PM2.5 来源解析技术及其应用 .404.2.1 两种源解析方法的比较 .404.2.2 受体模型的分类 .404.2.3 受体模型在我国 PM2.5 来源解析中的应用 .464.3 关中地区 PM2.5 来源解析 .474.3.1 PMF 源解析 .474.3.2 CMB 源解析 .544.3.3 PMF 和 CMB 解析结果对比 .594.4 解析结果对控制对策的指示意义 .614.4.1 燃煤管理意义 .614.4.2 机动车管理意义 .624.4.3 生物质燃烧管理意义 .634.4.4 地质尘管理意义 .63

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