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广西茅尾海底泥中氯代多环芳烃的研究

发布时间:2017-12-27 04:21

  本文关键词:广西茅尾海底泥中氯代多环芳烃的研究 出处:《上海大学》2016年硕士论文 论文类型:学位论文


  更多相关文章: 茅尾海 表层沉积物 氯代多环芳烃 正定矩阵模型


【摘要】:随着广西北部湾地区经济的快速发展,表层沉积物也成为影响茅尾海生态环境质量重要因素。结合国内外的相关研究,本研究以2014年4月采集的茅尾海表层沉积物为研究介质,系统研究了广西茅尾海表层沉积物样品中氯代多环芳烃(ClPAHs)的浓度水平、污染分布特征、来源解析、毒性当量及潜在污染源对目标污染物的毒性贡献。通过两种源解析方法对氯代多环芳烃的进行分析,更加详实了各污染源对氯代多环芳烃的环境浓度及毒性贡献。研究的结论如下:(1)本研究在茅尾海近岸海域总共布设35个采样站位,根据各区域地理地貌特征分为M、K、S和J四个区域。在所采集的表层沉积物样品(n=35)中,均检出了氯代多环芳烃,且20种目标氯代多环芳烃中有18种同系物被检出;这说明ClPAHs在该研究区域表层沉积物中已广泛存在。其中,∑Cl PAHs的浓度范围是0.31~9.64 ng/g dw,平均值为3.21 ng/g dw。其中6-ClBaP和9-ClPhe的平均浓度最高,与国内外关于表层沉积物中氯代多环芳烃的一致,这两种物质也是普遍偏高的。9-ClPhe的检出率为100%,平均浓度为1120.39 pg/g dw,高于氯代多环芳烃同系物。结合广西茅尾海形貌特征、产业框架和污染源等具体特点,通过与其他已有的少量的关于表层沉积物的文献报道的数据对比分析,可以推测广西茅尾海表层沉积物中ClPAHs的浓度水平在世界范围内属于中等水平。本研究中18种ClPAHs的总浓度随着采样点位置的不同,变化较大,这与茅尾海的特殊地貌和不同地点的附近污染源不同有关。茅尾海表层沉积物中ΣClPAHs浓度高值主要集中在J和K区,以及S地区一些采样点;其中K区的总浓度平均值(5.36 ng/g dw)最高,J区(4.22 ng/g dw)仅稍低于K区,浓度也是很高,M区的总浓度平均值(2.11 ng/g dw)最低。表明地理位置对表层沉积物中ClPAHs的空间分布有较为重要的影响。经过多方因素分析,石化工厂、水泥厂的复杂物质的排放,燃料燃烧和城市污水排放都是可能导致ClPAHs浓度高的原因。(2)本研究中利用REPBaPEC50/60使ClPAHs的毒性当量标准化,进而计算ClPAHs的总毒性当量。通过计算得到的氯代多环芳烃在广西茅尾海表层沉积物样品中的类二VA英总毒性当量(TEQClPAHs)为601.68 pg-TEQ/g,单体的毒性当量范围是2.32~185.97 pg-TEQ/g。按照ClPAHs同系物的TEQ排名为6-ClChr(30.91%)3,9,10-Cl3Phe(18.01%)7-ClBaA(15.77%)9-ClPhe(5.59%)9,10-Cl_2Phe(5.17%)6-ClBaP(4.33%)8-ClFlu(4.32%)7,12-Cl_2Ba A(2.53%)3-ClFlu(2.31%)。主要致癌物质为6-ClChr和3,9,10-Cl3Phe。对比国内外研究,表明广西茅尾海表层沉积物中ClPAHs对环境的毒性污染程度相对而言还是中等。(3)本研究选取6-ClBaP/1-ClPyr、3-ClFlu/1-ClPyr、6-ClBaP/3-ClFlu和1-ClPyr/3-ClFlu作为判断ClPAHs来源的标准。本文对比国内外研究并采用这种国际上广泛使用的特征比值法,分析发现广西茅尾海表层沉积物中的ClPAHs可能来自机动车尾气、垃圾焚烧、燃煤焚烧、化工工业生产等其他不确定污染源,即焚烧炉不完全燃烧的排放、交通尾气以及含氯材料的燃烧等。(4)利用PMF模型,本研究对广西茅尾海表层沉积物中的ClPAHs进行源解析,并对ClPAHs的每种来源的贡献进行计算,结果表明,与交通相关的污染物排放、石化工厂混合污染物的排放、林木和煤的燃烧和混合污染源(包括石化工厂的排放和城市日常废水及生活垃圾的排放)对ClPAHs浓度的源贡献分别是14.8%,18.6%,30.4%和36.2%。虽然PMF模型已经广泛用于环境分析中,但目前还没有报道用此正定矩阵模型研究广西茅尾海表层沉积物中的ClPAHs来源分布情况。为了更好的描述ClPAHs的毒性,本研究用正定矩阵因子模型结合毒性当量浓度,来定量的评估来自不同污染源的ClPAHs的毒性当量贡献值(TEQcontribution)。结果表明,交通相关的排放(0.47 pg TEQBaP g-1)、石化工厂的复杂排放物(0.92 pg TEQBaP g-1)、林木及煤的燃烧(1.06 pg TEQBaP g-1)和混合源(2.94 pg TEQBaP g-1)对ClPAHs的毒性效力是接近的,因此对这几个污染源的控制和治理,对改善广西茅尾海表层沉积物的质量非常重要。
[Abstract]:With the rapid economic development of Guangxi Beibu Gulf area, surface sediments also become an important factor affecting the quality of Maowei sea. Combining domestic and foreign relevant research, this study collected in April 2014 of Maowei Sea Surface Sediments of medium, studied chlorinated Guangxi Maowei Sea surface sediment samples of polycyclic aromatic hydrocarbons (ClPAHs) concentrations, pollution distribution, source analysis, toxicity when the quantity and toxicity of potential pollution source for target pollutant contribution. Two source analytical methods were used to analyze chloropolycyclic aromatic hydrocarbons, and the environmental concentration and toxicity of chloropolycyclic aromatic hydrocarbons (chloropolycyclic aromatic hydrocarbons) were more detailed. The conclusions are as follows: (1) this study in the coastal waters of Maowei Sea total layout 35 sampling stations, according to the regional geographic features is divided into M, K, S and J in four areas. Chlorinated polycyclic aromatic hydrocarbons (PAHs) were detected in the surface sediment samples (n=35) collected. 18 homologues were detected in 20 target chlorinated polycyclic aromatic hydrocarbons, indicating that ClPAHs has been widely distributed in the surface sediments of the study area. Among them, the concentration range of the sigma Cl PAHs is 0.31~9.64 ng/g DW with an average of 3.21 ng/g DW. The average concentration of 6-ClBaP and 9-ClPhe is the highest, which is the same as that of chloroaromatic hydrocarbons in the surface sediments. These two substances are also generally high. The detection rate of 9-ClPhe was 100%, and the average concentration was 1120.39 pg/g DW, which was higher than that of chloroaromatic hydrocarbon homologues. In combination with the specific characteristics of Guangxi Maowei morphology, industrial structure and pollution sources, by comparing the data with other existing small amounts on the surface sediments reported in the literature analysis, we can conclude that ClPAHs concentrations in the surface sediments of Maowei Sea Guangxi belongs to the medium level in the world. The total concentration of 18 ClPAHs in this study with the sampling points in different position, changes in the larger, and the special features of the Maowei Sea and different locations near the pollution sources related to the different. Maowei Sea Surface Sediments in the sigma ClPAHs concentration mainly concentrated in J and K area, S area and some sampling points; the average value of the total concentration of K (5.36 ng/g DW), J region (4.22 ng/g DW) only slightly lower than K, the concentration is very high, the average value of the total concentration of M the lowest (2.11 ng/g DW). It shows that the geographical location has a more important influence on the spatial distribution of ClPAHs in the surface sediments. After many factors analysis, the emissions of complex substances in petrochemical plants and cement plants, fuel combustion and urban sewage discharge all contribute to the high concentration of ClPAHs. (2) in this study, the toxicity equivalent of ClPAHs was normalized by REPBaPEC50/60, and the total toxicity equivalent of ClPAHs was calculated. Through the calculation of chlorinated polycyclic aromatic hydrocarbons in Guangxi Maowei Sea surface sediment samples in the two VA total toxic equivalent (TEQClPAHs) for 601.68 pg-TEQ/g, the toxic equivalent range of monomers is 2.32~185.97 pg-TEQ/g. According to the TEQ of ClPAHs homologues, the ranking is 6-ClChr (30.91%) 3,9,10-Cl3Phe (18.01%) 7-ClBaA (15.77%) 9-ClPhe (5.59%) 9,10-Cl_2Phe (5.17%) 6-ClBaP (4.33%) 8-ClFlu (4.32%) 7,12-Cl_2Ba A (2.53%) 3-ClFlu (2.31%). The main carcinogens are 6-ClChr and 3,9,10-Cl3Phe. The comparison of domestic and foreign research shows that the pollution degree of Maowei Sea Surface Sediment Toxicity of ClPAHs in Guangxi on the environment is still relatively moderate. (3) this study selected 6-ClBaP/1-ClPyr, 3-ClFlu/1-ClPyr, 6-ClBaP/3-ClFlu and 1-ClPyr/3-ClFlu as the criteria for judging the source of ClPAHs. This paper contrasts the domestic and foreign research and the characteristics of the ratio method is widely used. The analysis found that the sediment of Maowei Sea Surface in Guangxi in ClPAHs from motor vehicle exhaust, waste incineration, incineration, coal chemical industrial production and other uncertain sources of pollution, namely incinerator incomplete combustion emissions, vehicle exhaust and combustion of materials containing chlorine etc.. (4) using the PMF model, the ClPAHs on the surface sediments of Maowei Sea in Guangxi for source apportionment, and the ClPAHs of each source contributions are calculated, the results show that the emission of pollutants and petrochemical factories and traffic related pollutants emissions, forest and coal burning and mixed pollution sources (emissions and city the daily waste and garbage including petrochemical factory emissions) contribution to the concentration of ClPAHs source were 14.8%, 18.6%, 30.4% and 36.2%. Although the PMF model has been widely used in environmental analysis, but there is no research on the positive definite matrix model of Maowei Sea Surface Sediments reported in Guangxi ClPAHs source distribution. In order to better describe the toxicity of ClPAHs, we used the positive definite matrix factor model combined with the toxicity equivalent concentration to quantitatively evaluate the toxicity equivalent contribution value (TEQcontribution) of ClPAHs from different sources. The results show that the traffic related emission (0.47 PG TEQBaP g-1), complex emissions from petrochemical plants (0.92 PG TEQBaP g-1), timber and coal combustion (1.06 PG TEQBaP g-1) and mixed source (2.94 PG TEQBaP g-1) toxicity potency against ClPAHs is close, so a few of these pollution sources control and management, is very important to improve the quality of surface sediments of Maowei Sea in Guangxi.
【学位授予单位】:上海大学
【学位级别】:硕士
【学位授予年份】:2016
【分类号】:X55;X592

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