本文選題：多環(huán)芳烴 + 多氯聯(lián)苯��； 參考：《華東師范大學(xué)》2017年博士論文

【摘要】：多環(huán)芳烴(PAHs)和多氯聯(lián)苯(PCBs)是兩類典型的具有致癌、致畸和致突變的持久性有機污染物(POPs),可通過多種環(huán)境介質(zhì)進行長距離遷移,且對人類健康和環(huán)境安全具有嚴重危害。地表水體是PAHs、PCBs等污染物的重要的環(huán)境受體,因此研究PAHs、PCBs在典型地表水體中的暴露水平、環(huán)境行為及其造成的環(huán)境風(fēng)險具有重要的理論和現(xiàn)實意義。本研究在國家自然科學(xué)基金項目(No.41271472)、上海市科委社會發(fā)展重點項目(No.12231201900)的資助下,利用氣相色譜法/質(zhì)譜聯(lián)用技術(shù)(GC/MS)測定了上海市河網(wǎng)、滴水湖及其環(huán)湖水系水、沉積物中PAHs、PCBs的暴露濃度,運用統(tǒng)計學(xué)和GIS等方法分析了 PAHs和PCBs的污染水平與時空分布規(guī)律,利用冗余分析(RDA)等方法探討了 PAHs和PCBs的污染分布及分配行為與環(huán)境因子間的耦合關(guān)系,綜合主成分分析(PCA)、絕對主成分/多元線性回歸(APCS/MLR)及正定矩陣因子分解(PMF)等方法對比分析了其來源與來源貢獻率。在此基礎(chǔ)上,基于景觀用水用途的暴露情境,分析了 PAHs、PCBs對上海市成人、兒童造成的致癌性健康風(fēng)險和非致癌性健康風(fēng)險,結(jié)合美國國家環(huán)境保護局(USEPA)推薦的定量結(jié)構(gòu)-活性相關(guān)模型(QSAR)(ECOSAR)和北京大學(xué)開發(fā)的基于貝葉斯理論的風(fēng)險評估模型(BMC-SSD)推導(dǎo)了符合研究區(qū)水系、水體特征的水生生物預(yù)測無效應(yīng)濃度(PNEC),并利用商值法對其生態(tài)風(fēng)險水平進行了表征。得出的主要結(jié)論如下:(1)研究區(qū)表層水、沉積物中16種PAHs整體處于輕微至中度污染水平,各相中PAHs均以3～5環(huán)成分為主,含量較高的單體有Phe、Ant和Flua。表層水中PCBs為輕中度污染,而沉積物中PCBs為輕微污染,各相中PCBs均以五氯聯(lián)苯為主,主要的特征單體為PCB118、PCB105和PCB77。受河道水動力條件較弱、黑臭現(xiàn)象較嚴重等因素影響,中心城區(qū)以及城鎮(zhèn)居民區(qū)河網(wǎng)水體中PAHs、PCBs污染相對嚴重。滴水湖環(huán)湖水系水體中的PAHs、PCBs含量普遍高于湖區(qū)。除秋季沉積物中的PCBs外,冬季表層水中的PAHs和PCBs均顯著高于其他季節(jié)。(2)"鹽析效應(yīng)"、水質(zhì)現(xiàn)狀、總懸浮顆粒物(TSS)和溶解性有機質(zhì)(DOC)是影響水中PAHs、PCBs分布的重要因素。沉積物中PAHs分布受沉積物的機械組成和碳黑(SC)影響顯著,PCBs分布則受SC、TOC影響顯著。水溫、鹽度及水中的TSS、DOC對PAHs、PCBs在顆粒物-水間的分配行為影響較大。PAHs、PCBs的沉積物-水分配行為均受沉積物機械組成影響顯著,SOC及TOC含量對PAHs的沉積物-水分配行為影響顯著,但對PCBs的影響不顯著�，F(xiàn)場數(shù)據(jù)較好地擬合了沉積物-水中PAHs的分配行為,但并不能很好地擬合沉積物-水中PCBs的分配行為。(3)正定矩陣分解法(PMF)較之主成分分析法(PCA)和絕對主成分/多元線性回歸法(APCS/MLR)對PAHs源解析的結(jié)果更全面,源解析結(jié)果表明研究區(qū)地表水中PAHs主要來自于煤、薪柴和天然氣等燃燒源以及焦化源排放,而沉積物中的PAHs受交通源的貢獻最高,其次為燃燒源和焦化源。PCA法及PMF法均區(qū)分出了 PCBs的4類源,但貢獻率計算結(jié)果存在一定差異�？傮w而言,研究區(qū)地表水體中PCBs主要來自國產(chǎn)PCB工業(yè)品的使用殘留,但也受再生金屬加工行業(yè)排放以及國外PCB產(chǎn)品的使用殘留與遠距離輸送影響。(4)河網(wǎng)水體中PAHs、PCBs的成人的總致癌風(fēng)險水平已超過了最大可接受致癌風(fēng)險水平,兒童僅除崇明島及農(nóng)業(yè)區(qū)部分點位外,其他點位的總致癌風(fēng)險也均超過了最大可接受風(fēng)險水平。對于滴水湖及其環(huán)湖水系水體中PAHs、PCBs,僅有9.3%的點位成人總致癌風(fēng)險及18.67%的點位兒童總致癌風(fēng)險處于可接受水平。皮膚接觸是景觀用水暴露情境中PAHs、PCBs致癌風(fēng)險的主要暴露途徑,但不會造成明顯的非致癌健康傷害。(5)利用ECOSAR及BMC-SSD模型推導(dǎo)的預(yù)測無效應(yīng)濃度(PNEC)與其他研究具有較好的可比性。研究區(qū)存在較高生態(tài)風(fēng)險水平的PAHs單體主要有水中的苯并[b]熒蒽(BbF)、苯并[k]熒蒽(BkF)、BghiP以及沉積物中菲(Phe)、熒蒽(Flua)和芘(Pyr),存在高生態(tài)風(fēng)險水平的PAHs單體主要為Phe、蒽(Ant)、窟(Chry)、Flua和Pyr。水體中具有高生態(tài)風(fēng)險水平的DL-PCBs單體主要為溶解態(tài)中的PCB105、顆粒態(tài)中的PCB118、PCB105和PCB77。
[Abstract]:Polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) are two types of typical carcinogenic, teratogenic and mutagenic persistent organic pollutants (POPs), which can carry long distance migration through a variety of environmental mediums, and have serious harm to human health and environmental safety. Surface water is an important environmental receptor for PAHs, PCBs and other pollutants. Therefore, the study of PAH The exposure levels of S, PCBs in typical surface waters, environmental behavior and environmental risks are of great theoretical and practical significance. Under the support of the National Natural Science Foundation (No.41271472) and the key social development project (No.12231201900) of the Shanghai Municipal Science and Technology Commission (No.12231201900), this study was determined by gas chromatography / mass spectrometry (GC/MS). The pollution level and spatio-temporal distribution of PAHs and PCBs were analyzed by statistics and GIS, and the pollution distribution of PAHs and PCBs and the coupling relationship between the distribution behavior and environmental factors were discussed by the methods of redundancy analysis (RDA) and so on. The pollution distribution of PAHs and PCBs were analyzed by the methods of statistics and GIS, and the pollution levels of PAHs and PCBs in the sediments and the exposure concentration of the sediments were analyzed. Principal component analysis (PCA), absolute principal component / multivariate linear regression (APCS/MLR) and positive definite matrix factorization (PMF) were used to compare their source and source contribution rates. Based on the exposure scenarios of landscape water use, the carcinogenic health risks and non carcinogenic health risks caused by PAHs and PCBs for children in Shanghai City were analyzed. Combined with the quantitative structure activity correlation model (QSAR) (ECOSAR) recommended by the national environmental protection agency of the United States (USEPA) and the Bayesian based risk assessment model (BMC-SSD) developed by the Peking University (BMC-SSD), this paper derives the ineffective stress concentration (PNEC) of aquatic organisms in accordance with the water system and water characteristics in the study area, and uses the quotient method for its ecological wind. The main conclusions are as follows: (1) the surface water of the study area, 16 kinds of PAHs in the sediments are in the mild to moderate pollution level, and the PAHs in each phase is dominated by 3~5 ring components, the monomer with higher content is Phe, the PCBs in the surface water of Ant and Flua. is light medium pollution, and the PCBs in the sediments is slightly polluted and PCBs in each phase. The main characteristics are five chlorinated biphenyls, the main characteristic monomers are PCB118, PCB105 and PCB77. are influenced by the weak river hydrodynamic conditions and the serious black odor. The pollution of PAHs in the river net water of the central urban area and the urban residential area is relatively serious. The PAHs in the water system of the drip lake lake water system is generally higher than that in the lake area. Except for the autumn deposition, the content of PCBs is generally higher than that in the lake area. The PAHs and PCBs in surface water in winter are significantly higher than those of other seasons. (2) "salting out effect", water quality, total suspended particles (TSS) and dissolved organic matter (DOC) are important factors affecting the distribution of PAHs and PCBs in water. The PAHs distribution in the sediments is influenced significantly by the mechanical composition of the sediments and the carbon black (SC), while PCBs distribution is SC, TO. The effect of C on water temperature, salinity and TSS in water, DOC to PAHs, PCBs in the distribution of particles and water has great influence on.PAHs, and the sediment water distribution behavior of PCBs is greatly influenced by the mechanical composition of sediment, SOC and TOC content has a significant influence on the sediment water distribution behavior of PAHs, but the effect on PCBs is not significant. Field data is well proposed. The distribution behavior of PAHs in sediment water can not be well fitted to the distribution behavior of PCBs in the sediment water. (3) the positive definite matrix decomposition (PMF) is more comprehensive than the principal component analysis (PCA) and the absolute principal component / linear regression (APCS/MLR) for the analysis of PAHs source. The source analysis results show that the PAHs master in the surface water of the study area is dominant. It is derived from coal, firewood, natural gas and other combustion sources, as well as the source of coking source, and the PAHs in the sediment is the highest contribution to the traffic source. Secondly, the 4 sources of PCBs are separated from the combustion source, the focal.PCA method and the PMF method, but the calculation results of the contribution rate are different. In general, the PCBs in the surface water of the study area is mainly from the domestic PC. The use of B industrial products remains, but it is also affected by regenerated metal processing industry emissions and the use of residual and remote delivery of foreign PCB products. (4) the total cancer risk level for adults of PAHs, PCBs in river network waters has exceeded the maximum acceptable level of carcinogenic risk. Children are only in addition to some points in Chongming Island and agricultural areas, and the total number of other points. The risk of carcinogenesis also exceeded the maximum acceptable risk level. For PAHs, PCBs, only 9.3% of the total oncogenic risk and 18.67% of the total oncogenic risk of children in the water drops lake and its lake water system, skin contact is the main way of exposure of PAHs, PCBs cancer risk in the landscape water exposure situation, but not (5) the predicted ineffective concentration (PNEC) derived from the ECOSAR and BMC-SSD models has better comparability with other studies. The high ecological risk levels of PAHs monomers in the study area are mainly benzene and [b] fluoranthene (BbF), benzo [k] fluoranthene (BkF), BghiP, and phenanthrene (Phe), fluoranthene (F). Lua) and pyrene (Pyr), the PAHs monomers with high ecological risk level are mainly Phe, anthracene (Ant), grottoes (Chry), and DL-PCBs monomers with high ecological risk in Flua and Pyr. water bodies are mainly PCB105 in the dissolved state, PCB118, PCB105 and minerals in the granular state.
【學(xué)位授予單位】：華東師范大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2017
【分類號】：X52

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