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辽河口湿地土壤中多环芳烃的分布特征及来源解析.pdf

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谨以此文献给所有曾经关心和帮助我的人l▲l-Ix,lI 一J■■■■■■■一lfll l 1 11 1 1 1 III I II II III\1 927274辽河口湿地土壤中多环芳烃的分布特征及来源解析答辩委员会成员签字一 眼雌独创 声 明本人声明所呈交的学位论文是本人在导师指导下进行的研究工作及取得的研究成果。据我所知,除了文中特别加以标注和致谢的地方外,论文中不包含其他人已经发表或撰写过的研究成果, 也不包含未获得注如没有其他需要特别声明的,本栏可空或其他教育机构的学位或证书使用过的材料。与我一同工作的同志对本研究所做的任何贡献均已在论文中作了明确的说明并表示谢意。学位论文作者签名力裂韦出k签字日期如厂,年6,q 7日学位论文版权使用授权书本学位论文作者完全了解学校有关保留、使用学位论文的规定,并同意以下事项1、学校有权保留并向国家有关部门或机构送交论文的复印件和磁盘,允许论文被查阅和借阅。2、学校可以将学位论文的全部或部分内容编入有关数据库进行检索,可以采用影印、缩印或扫描等复制手段保存、汇编学位论文。同时授权清华大学“中国学术期刊光盘版电子杂志社“用于出版和编入CNKI中国知识资源总库,授权中国科学技术信息研究所将本学位论文收录到中国学位论文全文数据库。保密的学位论文在解密后适用本授权书学位论文作者签名 态弗林 翩签字狮为签字日期动,/年‘月7日 签字日期Q轫J年占月9日辽河口湿地土壤中多环芳烃的分布特征及来源解析摘 要对辽河口湿地表层土壤中16种PAHs的含量进行分析,研究探讨了湿地非退化区和退化区中PAHs的分布特征。通过比值法定性解析了辽河口湿地表层土壤PAHs来源,并在此基础上进一步利用正定矩阵因子分解模型PMF和因子分析/多元线性回归模型FA仆嗄R对表层土壤中PAHs来源进行定量解析。这项工作对于了解辽河口湿地土壤PAHs的污染状况及时空分布,追踪其主要污染物来源具有重要指导意义。辽河口湿地31个站位的表层土壤样品中PAHs总量范围为293.4~1936.9ng/g,平均值为851.5 ng/g,与国内外河口湿地区域相比处于中等偏上的污染水平。各站位的NaP、Phe、Acy、Pyr、Fla、Ace、Fle含量较高,超过了16种优控PAHs总量的65%,高环PAHs的含量相对较低,占16种PAHs的20.8%。在非退化区中,不同时间PAHs总量大小顺序为2008年10月2009年05月2009年8月,三个季节的环数构成均表现为低环中环高环。不同类型非退化区PAHs含量差异明显,滩涂区PAils含量显著低于芦苇区,但是两者的环数构成比例比较相近。非退化区土壤PAHs含量与pH值、盐度和油类含量之间的相关性系数很低,与有机质、粘粒有较高的相关性。在退化区中,不同时间PAHs总量的大小顺序为2008年10月2009年05月2009年8月,三个季节的环数构成均表现为低环中环高环。翅碱蓬退化区和芦苇退化区的PAHs总量较为相近,均小于油井区苇田的PAHs含量。不同类型退化区的PAHs均是以低环组分为主,其中油井区PAHs污染表现出了明显的油类泄漏特征。退化区土壤PAHs总量与pH值、盐度之间的相关性系数很低,与有机质、粘粒和油类有较高的相关性。利用比值法对辽河口湿地表层土壤中PAHs进行定性源解析。研究发现,2008年lO月的PAHs污染主要为燃烧源,包括油类燃烧汽油燃烧与柴油燃烧、生物质燃烧以及煤的燃烧;2009年5月和8月的PAHs污染主要为混合源,包括石油类污染、油类燃烧以及生物质和煤燃烧。基于Spss 13.0软件,应用FA/MLR模型解析PAHs来源,结果显示2008年10月主要的PAHs污染源为燃煤/交通混合源44.4%、石油/交通混合源37.1%、燃煤源18.5%;2009年5月石油/交通的混合源74.8%、燃煤18.5%、交通污染6.7%;2009年8月石油/交通的混合源41.4%、交通污染36.4%和燃煤22.2%。PMF模型解析结果表明,2008年10月中,燃烧源是其主要来源,相对贡献率达到了47.6%,石油污染、交通燃油和炼焦的贡献相对较低,分别为17.9%、20.0%和14.5%。在2009年5月中,石油/交通污染的贡献率最大,为32.2%,其余三种污染源的贡献率分别为燃煤28.8%、石油污染24.6%、炼焦14.4%。2009年8月以石油污染和交通污染贡献率最高,贡献率分别为37.6%和32.7%,炼焦和燃煤的贡献率仅有13.8%和15.9%。综合两定量模型的结果发现,燃煤、交通污染、石油污染和焦炉源是辽河口湿地土壤PAl-Is的四类主要来源,其中2008年10月以燃煤和交通污染主,2009年5月和8月都是以石油和交通污染为最主要的污染源。关键词多环芳烃分布特征;河口湿地;因子分析/多元线性回归;正定矩阵因子分解模型 ’卫D i str i but i on and Sources Apport i onment of PAHs fromL i ‘ Estua i Re Wet I and Soaohekstua r et and 50 i I SL I I I l lAbstract1 6 polycyclic aromatic hydrocarbonsPAHswel“e measured by GCFID for3 1 surface soil samples collected from Liaohe estuary wetland in October 2008,Mayand August 2009.The distribution of PAi ls in soil in the degraded and non..degradedfrom Liaohe estuarine wetland W el e investigated in this article.The positive matrixfactorizationPMFand Factor analysis-multiple linear regression analysisFA-MLRwere used to quantitatively apportion sources of PAHs in surfac宅soils on the basis ofdiagnostic ratio analysis conclusion.This work would play an important role inunderstanding the pollution levels and distribution of PAHs in soil and tracking themain PAHs sources in Liaohe estuarine wetland.The results showed that the total concentrations of PAHs in surfac2 soil rangedfrom 293.4 to 1936.9 ng·g~with a mean of 851.5 ng.g~,which is at above theaverage level of PAHs pollutions compared with relevant areas worldwide.Theconcentrations of NaP,Phe,Aey,Pyr,Fla,Ace and FIe in different stations were athigher levels,which accounted for more than 65%of the total PAHs contents,whilethe proportion of the high molecular weight Was relatively low,accounting for 20.8%.In the un-degraded areas,the sequence of PAHs concentrations in different seasonsWas October 2008May 2009August 2009.The proportion of low molecularweight is higher than median and high molecular weight in three seasons.Thecontents of PAHs in the reed field were higher than beach,while the constitute ofPAHs rings in two types were similar.There were no correlations between PAHsconcentrations and pH,salinity and oil contents,whereas significant correlations werefound between PAi ls contents and organic matter and clay.In the degraded areas,the order of PAHs concentrations in different seasons isOctober 2008May 2009August 2009.nle proportion of low molecular weight ishigher than median and high molecular weight in three seasons.The contents of PAHsin the oil well reed field were higher than Suacda heteroptera degraded area and reedUldegraded area.The proportions of PAHs were dominated by low molecular weight ihthree degraded areas,and the oil well reed field showed the feature of oil spillpollution.There were no correlations between PAI ls concentrations and pH andsalinity,whereas significant correlations were found between PAi ls contents andorganic matter,clay and oil contents.Diagnostic ratio analysis illustrated that pyrolysis Was the main source of PAi lsin October 2008,including oil combustiongasoline combustion and dieselcombustion,biomass burning and coal combustion;while the mixed pollution ofpyrolysis and oil spill w勰the dominant PAi ls SOUl“Ce in May and August 2009.including oil pollution,oil combustion as well as biomass and coal combustion.Based on Spss 13.0 soth,vare,FA/MLR modal Was applied to identify the PAHsSOUrCeS.The results showed that the major source in October 2008 was coal/vehicularemission,oiYtraffic emission and coal combustion,、l,ith contributions of and 44.4%,37.1%and 1 8.5%.While the mixture of vehicular exhaust and oil spill Was the majorSOUl C 七in May and August 2009accounted for 74.8%and 41.4%respectively..PMF model Was also used to quantitatively analyze the m.ain PAi ls sources inLiaohe estuary wetlands.The result indicated that the main SOUrCeS of PAHs werecoal combustion,oil spill,traffic emission and coke oven in October 2008,诵也contributions of 47.6%,1 7.9%and 20.O%and 1 4.5%,respectively.Oil/trafficemission,coal combustion,oil spill and coke oven,丽也contributions of 32.2%,28.8%,24.6%and 14.4%,respectively,were the main PAH source-s in May 2009.InAugust 2009,oil spill埘m a contribution of 37.6%was dominant,followed by trafficemission,coke OVen and coal combustion,wi也contributiOIlS of 32.7%,1 3.8%,and1 5.9%,respectively.There were some differences between the two models results,and PMF model’S result was more suitable for the actual pollutions in Liaohe骼tuarywetl锄ds.There were some differences between the two models results,and the PMFmodel’S result Was more suitable for the actual pollutions in Liaohe estuary wetlands.Comparing the two results from different models,we know that coal combustion,traffic emission,oil spill and coke OVen were the SOUl GCS of PAHs in soils fromLiaohe e舭lrine wctland.The coal combustion and traffic emission dominated inIV
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