上海快速城市化進(jìn)程對多環(huán)芳烴湖泊沉積演變的影響研究
發(fā)布時(shí)間：2018-08-27 05:59
【摘要】：上海近百年來的快速城市化進(jìn)程,帶來人口的急劇增長,同時(shí)也帶來了一系列的環(huán)境污染問題,阻礙了社會、經(jīng)濟(jì)與環(huán)境的可持續(xù)發(fā)展。多環(huán)芳烴(Polycyclic aromatic hydrocarbons,PAHs)是一種持久性有機(jī)污染物,有較強(qiáng)的致癌、致畸、致突變的效應(yīng),普遍存在于環(huán)境各介質(zhì)中并且能進(jìn)行長距離遷移,對環(huán)境生態(tài)危害極大。本研究將從城市化與環(huán)境污染關(guān)系的角度出發(fā),通過分析上海城市公園湖泊沉積物中的PAHs,系統(tǒng)探討了其在不同時(shí)間和空間樣品中的含量與特征、來源、生態(tài)風(fēng)險(xiǎn),分析城市土地利用/土地覆被變化(LUCC)對表層沉積物PAHs賦存的影響,探究影響多環(huán)芳烴沉積的主要城市化參數(shù)及其作用機(jī)理,為控制城市化過程中的環(huán)境污染提供科學(xué)建議。表層沉積物樣品采自上海市4個(gè)城市化區(qū)域32個(gè)公園湖泊,即核心城區(qū)(CUC,位于內(nèi)環(huán)以內(nèi))、發(fā)達(dá)城區(qū)(DDU,位于內(nèi)環(huán)和中環(huán)之間)、發(fā)展中城區(qū)(DIU,位于中環(huán)和外環(huán)之間)和郊區(qū)(SU,外環(huán)以外)。三沉積柱樣品分別采自位于虹口區(qū)的魯迅公園(C1)和楊浦區(qū)的復(fù)興島公園(C2)與新江灣濕地公園(C3)。研究分析得到如下幾點(diǎn)認(rèn)識:上海公園湖泊表層沉積物中16種PAHs總濃度范圍是55.75-4928 ng/g,均值為1133ng/g。單因素方差分析結(jié)果表明各單體PAHs濃度在城市化區(qū)域之間差異較顯著(p0.05),呈現(xiàn)出由核心城區(qū)向郊區(qū)逐漸遞減的趨勢,高值點(diǎn)主要出現(xiàn)在核心城區(qū)交通人口密集區(qū)、浦西老工業(yè)區(qū)和郊區(qū)新興工業(yè)區(qū)附近。各采樣點(diǎn)多環(huán)芳烴組分均以4環(huán)濃度為最高,各區(qū)域之間除2環(huán)以外,3環(huán)、4環(huán)、5環(huán)和6環(huán)的濃度均值核心城區(qū)均大于其他區(qū)域,郊區(qū)為最低。基于PAHs總濃度的風(fēng)險(xiǎn)評價(jià)表明,表層沉積物中TEQ濃度范圍為3.42 ng/g-751.2 ng/g,PAHs毒性當(dāng)量濃度變化情況整體呈現(xiàn)出CUCDDUDIUSU,濃度最高值出現(xiàn)在位于核心城區(qū)的魯迅公園(S1)�；陲L(fēng)險(xiǎn)熵(RQ)的風(fēng)險(xiǎn)評估結(jié)果表明,單體Flu為高生態(tài)風(fēng)險(xiǎn),核心城區(qū)的公園湖泊沉積物PAHs的生態(tài)風(fēng)險(xiǎn)最高,發(fā)達(dá)城區(qū)和發(fā)展中城區(qū)為中等生態(tài)風(fēng)險(xiǎn)等級,郊區(qū)生態(tài)風(fēng)險(xiǎn)水平較低。城市LUCC對表層沉積物中PAHs賦存影響分析中,基于土地利用要素和PAHs濃度數(shù)據(jù)構(gòu)建的土地利用回歸(LUR)模型揭示了交通擁堵指數(shù)和工業(yè)點(diǎn)源個(gè)數(shù)對 PAHs 的顯著貢獻(xiàn),以 ∑16PAHs、∑2ringPAHs、∑3ringPAHs、∑4ringPAHs、∑5ringPAHs和∑6ringPAHs濃度為因變量構(gòu)建的LUR模型調(diào)整后的R2分別為0.984、0.529、0.979、0.977、0.974和0.943,三模型交叉檢驗(yàn)擬合的PAHs濃度與實(shí)測濃度之間均顯著相關(guān)(p0.01),相關(guān)系數(shù)分別為0.766、0.679、0.728、0.702、0.715、0.761,RMSE 值分別為 0.362、0.342、0.317、0.447、0.410、0.423。說明構(gòu)建的模型能較好的模擬了 PAHs濃度的空間分布特征。~(210)Pb和~(137)Cs聯(lián)合定年法結(jié)果表明C1、C2和C3沉積柱分別記錄了 1761-2012、1861-2012和1779-2012年間多環(huán)芳烴的沉積特征。三沉積柱中∑16PAHs和強(qiáng)致癌∑7PAHs的沉積通量隨著時(shí)間推進(jìn)均呈現(xiàn)出波動式增長,尤其是在1949年新中國成立以后和1978年改革開放以后有明顯的加速累積過程。經(jīng)沉積物聚集因子校正后的三沉積柱中∑16PAHs沉積通量和人為沉積通量均值分別為96.03、88.68、220.4 ng/cm2/yr 和 91.80、109.6、280.5 ng/cm2/yr,強(qiáng)致癌∑7PAHs沉積通量和人為沉積通量均值分別為55.82、53.06、125.2 ng/cm2/yr和109.2、65.53、159.5 ng/cm2/yr。2000 年后三沉積柱中∑16PAHs(強(qiáng)致癌∑7PAHs)平均人為沉積通量比值高達(dá) 162.74(194.62)、98.82(98.95)、356.78(394.57)。較高的通量比值說明公園湖泊PAHs的歷史沉積受到人類活動的強(qiáng)烈影響,C3沉積柱人為沉積通量校準(zhǔn)后的數(shù)值顯著增加可能與其所在的區(qū)域的周邊環(huán)境和本身的地域特征有關(guān)。利用正定矩陣因子(PMF)對表層湖泊沉積物進(jìn)行源解析表明結(jié)果PAHs來源主要是交通源和煤及生物質(zhì)的燃燒,采用特征比值法對沉積柱中的多環(huán)芳烴的來源解析,主要來自熱解源(主要是化石燃料和生物質(zhì)的燃燒),其中城市交通源也是主要來源。進(jìn)一步對城市化參數(shù)與多環(huán)芳烴沉積的相關(guān)性分析發(fā)現(xiàn),上海城市公園多環(huán)芳烴湖泊沉積污染格局的形成與演變與城市人口集聚、經(jīng)濟(jì)發(fā)展水平、能源消耗和產(chǎn)業(yè)結(jié)構(gòu)等因素關(guān)系緊密。從人口、經(jīng)濟(jì)和技術(shù)角度構(gòu)建了擴(kuò)展的隨機(jī)影響模型(STIRPAT)并定量解析了城市化參數(shù)對多環(huán)芳烴沉積的貢獻(xiàn)率,結(jié)果表明了人口總數(shù)、重工業(yè)比例和煤炭消耗量是多環(huán)芳烴沉積的主要影響因素,這三個(gè)指標(biāo)每提高1%,多環(huán)芳烴通量分別增加0.172%-0.198%、0.314%-0.358%和0.297%-0.308%。通徑分析結(jié)果也表明人口總數(shù)、重工業(yè)比例和煤炭消耗量對PAHs沉積的直接和間接影響都比較大。
[Abstract]:The rapid urbanization of Shanghai in the past century has brought about a rapid increase in population and a series of environmental pollution problems, hindering the sustainable development of society, economy and environment. Polycyclic aromatic hydrocarbons (PAHs) are a kind of persistent organic pollutants with strong carcinogenic, teratogenic and mutagenic effects. In this study, PAHs in lake sediments of urban parks in Shanghai were analyzed from the point of view of the relationship between urbanization and environmental pollution, and their contents, characteristics, sources and ecological risks in different time and space samples were systematically discussed. The effects of land use/land cover change (LUCC) on the occurrence of PAHs in surface sediments were analyzed, and the main urbanization parameters affecting PAHs deposition and their mechanisms were explored. Scientific suggestions were provided for controlling environmental pollution during urbanization. Core urban area (CUC, located within the inner ring), developed urban area (DDU, located between the inner and middle ring), developing urban area (DIU, located between the central and outer ring) and suburban area (SU, outside the outer ring). Three sediment column samples were collected from Luxun Park (C1) in Hongkou District and Fuxing Island Park (C2) and Xinjiangwan Wetland Park (C3) in Yangpu District, respectively. The results showed that the total PAHs concentration ranged from 55.75 ng/g to 4928 ng/g and the mean value was 1133 ng/g in the surface sediments of the lakes in Shanghai Park. The results of one-way ANOVA analysis showed that the PAHs concentration of each monomer was significantly different among the urbanized areas (p0.05), showing a gradual decrease trend from the core urban area to the suburbs, and the high-value points mainly appeared. The concentrations of PAHs in the four rings were the highest in all sampling sites. The mean concentrations of PAHs in the three rings, three rings, four rings, five rings and six rings were higher in the core city than in other areas, and the lowest in the suburbs. The concentration range of TEQ in surface sediments was 3.42 ng/g-751.2 ng/g. The variation of PAHs toxicity equivalent concentration showed CUCDDUDIUSU as a whole. The highest concentration appeared in Luxun Park (S1) located in the core city. Risk assessment based on risk entropy (RQ) showed that flu was a high ecological risk, and PAHs in park lake sediments in the core city was a high ecological risk. In the analysis of the influence of urban LUCC on the occurrence of PAHs in surface sediments, the land use regression (LUR) model based on land use factors and PAHs concentration data reveals that the traffic congestion index and the number of industrial sources affect P The significant contributions of AHs were as follows: the adjusted R2 values of LUR models were 0.984, 0.529, 0.979, 0.977, 0.974 and 0.943, respectively, with 16 PAHs, 2 ringPAHs, 3 ringPAHs, 4 ringPAHs, 5 ringPAHs, and 6 ringPAHs as dependent variables. The values of RMSE were 0.362, 0.342, 0.317, 0.447, 0.410, 0.423, respectively. The results show that the model can well simulate the spatial distribution characteristics of PAHs concentration. ~ (210) Pb and ~ (137) Cs dating results show that C1, C2 and C3 sedimentary columns recorded 1761-2012, 1861-2012 and 1779-2012, respectively. The deposition fluxes of 16PAHs and 7PAHs in the three sediment columns showed a fluctuating increase with time, especially after the founding of New China in 1949 and the reform and opening up in 1978. The 16PAHs deposition fluxes and human activities in the three sediment columns corrected by the sediment accumulation factor. The mean deposition fluxes of 7PAHs and anthropogenic fluxes were 96.03, 88.68, 220.4 ng/cm 2/yr and 91.80, 109.6, 280.5 ng/cm 2/yr, respectively. The mean deposition fluxes of 7PAHs and anthropogenic fluxes were 55.82, 53.06, 125.2 ng/cm 2/yr and 109.2, 65.53, 159.5 ng/cm 2/yr in the three deposition columns after 2000. The high flux ratios indicate that the historical deposition of PAHs in the park lake is strongly influenced by human activities. The significant increase of anthropogenic deposition flux in the C3 sediment column after calibration may be related to the surrounding environment and the regional characteristics of the area in which the PAHs are located. PMF) Source analysis of surface lake sediments shows that PAHs are mainly from traffic sources and combustion of coal and biomass. The source of PAHs in sediment columns is mainly from pyrolysis sources (mainly from combustion of fossil fuels and biomass), and urban traffic sources are also the main sources. The correlation analysis between urbanization parameters and PAH deposition shows that the formation and evolution of PAH lake sediment pollution pattern in Shanghai urban parks are closely related to urban population agglomeration, economic development level, energy consumption and industrial structure. The contribution rate of urbanization parameters to PAHs deposition was analyzed quantitatively. The results showed that population, heavy industry ratio and coal consumption were the main factors affecting PAHs deposition. For each increase of 1%, the flux of PAHs increased by 0.172% - 0.198%, 0.314% - 0.358% and 0.297% - 0.308% respectively. The total number of mouth, heavy industry and coal consumption had direct and indirect effects on PAHs deposition.
【學(xué)位授予單位】：華東師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：X524
本文編號：2206325
[Abstract]:The rapid urbanization of Shanghai in the past century has brought about a rapid increase in population and a series of environmental pollution problems, hindering the sustainable development of society, economy and environment. Polycyclic aromatic hydrocarbons (PAHs) are a kind of persistent organic pollutants with strong carcinogenic, teratogenic and mutagenic effects. In this study, PAHs in lake sediments of urban parks in Shanghai were analyzed from the point of view of the relationship between urbanization and environmental pollution, and their contents, characteristics, sources and ecological risks in different time and space samples were systematically discussed. The effects of land use/land cover change (LUCC) on the occurrence of PAHs in surface sediments were analyzed, and the main urbanization parameters affecting PAHs deposition and their mechanisms were explored. Scientific suggestions were provided for controlling environmental pollution during urbanization. Core urban area (CUC, located within the inner ring), developed urban area (DDU, located between the inner and middle ring), developing urban area (DIU, located between the central and outer ring) and suburban area (SU, outside the outer ring). Three sediment column samples were collected from Luxun Park (C1) in Hongkou District and Fuxing Island Park (C2) and Xinjiangwan Wetland Park (C3) in Yangpu District, respectively. The results showed that the total PAHs concentration ranged from 55.75 ng/g to 4928 ng/g and the mean value was 1133 ng/g in the surface sediments of the lakes in Shanghai Park. The results of one-way ANOVA analysis showed that the PAHs concentration of each monomer was significantly different among the urbanized areas (p0.05), showing a gradual decrease trend from the core urban area to the suburbs, and the high-value points mainly appeared. The concentrations of PAHs in the four rings were the highest in all sampling sites. The mean concentrations of PAHs in the three rings, three rings, four rings, five rings and six rings were higher in the core city than in other areas, and the lowest in the suburbs. The concentration range of TEQ in surface sediments was 3.42 ng/g-751.2 ng/g. The variation of PAHs toxicity equivalent concentration showed CUCDDUDIUSU as a whole. The highest concentration appeared in Luxun Park (S1) located in the core city. Risk assessment based on risk entropy (RQ) showed that flu was a high ecological risk, and PAHs in park lake sediments in the core city was a high ecological risk. In the analysis of the influence of urban LUCC on the occurrence of PAHs in surface sediments, the land use regression (LUR) model based on land use factors and PAHs concentration data reveals that the traffic congestion index and the number of industrial sources affect P The significant contributions of AHs were as follows: the adjusted R2 values of LUR models were 0.984, 0.529, 0.979, 0.977, 0.974 and 0.943, respectively, with 16 PAHs, 2 ringPAHs, 3 ringPAHs, 4 ringPAHs, 5 ringPAHs, and 6 ringPAHs as dependent variables. The values of RMSE were 0.362, 0.342, 0.317, 0.447, 0.410, 0.423, respectively. The results show that the model can well simulate the spatial distribution characteristics of PAHs concentration. ~ (210) Pb and ~ (137) Cs dating results show that C1, C2 and C3 sedimentary columns recorded 1761-2012, 1861-2012 and 1779-2012, respectively. The deposition fluxes of 16PAHs and 7PAHs in the three sediment columns showed a fluctuating increase with time, especially after the founding of New China in 1949 and the reform and opening up in 1978. The 16PAHs deposition fluxes and human activities in the three sediment columns corrected by the sediment accumulation factor. The mean deposition fluxes of 7PAHs and anthropogenic fluxes were 96.03, 88.68, 220.4 ng/cm 2/yr and 91.80, 109.6, 280.5 ng/cm 2/yr, respectively. The mean deposition fluxes of 7PAHs and anthropogenic fluxes were 55.82, 53.06, 125.2 ng/cm 2/yr and 109.2, 65.53, 159.5 ng/cm 2/yr in the three deposition columns after 2000. The high flux ratios indicate that the historical deposition of PAHs in the park lake is strongly influenced by human activities. The significant increase of anthropogenic deposition flux in the C3 sediment column after calibration may be related to the surrounding environment and the regional characteristics of the area in which the PAHs are located. PMF) Source analysis of surface lake sediments shows that PAHs are mainly from traffic sources and combustion of coal and biomass. The source of PAHs in sediment columns is mainly from pyrolysis sources (mainly from combustion of fossil fuels and biomass), and urban traffic sources are also the main sources. The correlation analysis between urbanization parameters and PAH deposition shows that the formation and evolution of PAH lake sediment pollution pattern in Shanghai urban parks are closely related to urban population agglomeration, economic development level, energy consumption and industrial structure. The contribution rate of urbanization parameters to PAHs deposition was analyzed quantitatively. The results showed that population, heavy industry ratio and coal consumption were the main factors affecting PAHs deposition. For each increase of 1%, the flux of PAHs increased by 0.172% - 0.198%, 0.314% - 0.358% and 0.297% - 0.308% respectively. The total number of mouth, heavy industry and coal consumption had direct and indirect effects on PAHs deposition.
【學(xué)位授予單位】：華東師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：X524
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