本文選題：多環(huán)芳烴 + 沉積物��； 參考：《南京大學(xué)》2017年碩士論文

【摘要】：流域-河口-近海系統(tǒng)受到陸地與海洋的共同影響,系統(tǒng)內(nèi)存在復(fù)雜的物理化學(xué)過程,是一個(gè)極其脆弱的生態(tài)系統(tǒng)。此外,社會(huì)經(jīng)濟(jì)的發(fā)展使得該區(qū)域還面臨巨大的人類活動(dòng)壓力,大量的污染物被排放到該區(qū)域,使得系統(tǒng)內(nèi)的生態(tài)和環(huán)境受到了極大的破壞。因此,對(duì)于該系統(tǒng)內(nèi)污染物環(huán)境行為方面的研究變得十分重要和緊迫。本研究以長(zhǎng)江流域-河口-近海環(huán)境作為典型研究區(qū)域,分析系統(tǒng)內(nèi)持久性有機(jī)污染物——多環(huán)芳烴(Polycyclic aromatic hydrocarbons,PAHs)的賦存情況,揭示系統(tǒng)內(nèi)PAHs的來源、分布和組成情況,深入探究該系統(tǒng)內(nèi)PAHs環(huán)境行為的可能性影響因素。長(zhǎng)江全流域表層水體中溶解相PAHs(DPAHs)的濃度范圍為17.7ng/L～110 ng/L,平均值為42.6ng/L。整體看來,流域由上游到下游PAHs具有明顯的累積遞增的趨勢(shì),但是三峽水庫出現(xiàn)明顯低值,其對(duì)于流域DPAHs具有明顯的調(diào)節(jié)作用。這可能是由于三峽水庫的蓄水功能對(duì)于PAHs具有一定的沖淡效應(yīng)。流域水體中主要以低環(huán)PAHs(2-3環(huán))為主,其含量約為水體中總DPAHs含量的67%。源解析結(jié)果顯示,流域水體中PAHs主要有四種來源:生物質(zhì)燃料和煤炭燃燒混合源,石油類物質(zhì)泄漏源,交通混合源(柴油和汽油發(fā)動(dòng)機(jī))和焦炭源,各污染源的貢獻(xiàn)率分別為40.1%、19.6%、17.5%和22.8%。長(zhǎng)江中下游流域水體中懸浮顆粒相PAHs(PPAHs)的濃度分布范圍為595.91 ng/g—2473.74ng/g(干重),平均濃度約為1369.92ng/g。兩湖(洞庭湖和鄱陽湖)出現(xiàn)濃度高值,自兩湖往下游PPAHs濃度同樣出現(xiàn)累積遞增趨勢(shì)。兩湖由于自身的匯水功能,且流域均屬于經(jīng)濟(jì)快速發(fā)展地區(qū),因此,其對(duì)PAHs具有一定的匯聚功能。下游河段(自九江站至常熟站)水體中PPAHs含量表現(xiàn)出較為明顯的累積效應(yīng),尤其是在鎮(zhèn)江站出現(xiàn)了最高值。而在常熟站監(jiān)測(cè)到的PPAHs濃度較鎮(zhèn)江站和南京站出現(xiàn)了明顯偏低的現(xiàn)象,可能是由于該站位靠近河口地區(qū)受到河口潮流的影響,對(duì)該站位水體中PPAHs具有一定的沖淡效應(yīng)。中下游河段PPAHs主要是以高分子量為主(4-6環(huán)),占據(jù)了 PAHs總量的84%以上。長(zhǎng)江口及其鄰近海域表層沉積物中PAHs的總濃度范圍處于26.6-621.6 ng/g(干重)之間,平均濃度約為158.2ng/g�？傮w看來,PAHs在空間上的分布具有很大的差異性,可將其分為兩個(gè)部分:長(zhǎng)江口區(qū)域和杭州灣南部的浙江近岸海域,濃度的高值區(qū)出現(xiàn)在杭州灣外的舟山群島以東海域。長(zhǎng)江口區(qū)域表層沉積物中PAHs的濃度范圍處于27.2-400.9ng/g,平均濃度大約為137.7ng/g;而鄰近浙江近岸海域表層沉積物中PAHs的濃度處于27.3-621.6 ng/g,平均濃度約為175.8 ng/g�？臻g上,PAHs的濃度分布具有由北往南逐漸升高的趨勢(shì),這與研究區(qū)沉積物粒度粒度的變化趨勢(shì)較為一致。此外,PAHs的濃度還存在由河口向外海先逐漸減小后逐漸變大的趨勢(shì),這可能受河口地區(qū)復(fù)雜的水動(dòng)力條件的影響。長(zhǎng)江泥沙進(jìn)入河口后,由于咸淡水混合和潮流的頂托作用在河口地區(qū)發(fā)生堆積。此外,河口區(qū)繁忙的航運(yùn)活動(dòng)產(chǎn)生大量的PAHs也在河口區(qū)發(fā)生沉降,使得河口區(qū)PAHs出現(xiàn)高值區(qū)。然而,河口地區(qū)強(qiáng)勁的動(dòng)力尤其是長(zhǎng)江沖淡水使得大量的PAHs被帶到較遠(yuǎn)的口外地區(qū),在搬運(yùn)過程中隨著沉積物一起發(fā)生分選和堆積,最終大量的PAHs與細(xì)顆粒沉積物在長(zhǎng)江口泥質(zhì)區(qū)發(fā)生堆積,使得該區(qū)域PAHs出現(xiàn)濃度高值。整個(gè)研究區(qū)中高分子量PAHs的濃度范圍約在12.9-436.3 ng/g,大約占據(jù)了 PAHs總濃度的30.3%-89%。研究區(qū)內(nèi)PAHs濃度與沉積物粒度和有機(jī)碳含量的分布特征具有一定的相似性,然而,相關(guān)性分析結(jié)果表明三者之間的相關(guān)性并不明顯。這可能是由于PAHs的吸附行為是一個(gè)復(fù)雜的過程,沉積物粒度和有機(jī)碳對(duì)其均有吸附偏好,且該區(qū)域強(qiáng)勁的動(dòng)力條件也會(huì)使得PAHs發(fā)生再分配。因此,復(fù)雜的控制因素使得三者之間的相關(guān)關(guān)系變得模糊。源解析結(jié)果顯示該研究區(qū)PAHs主要來自于煤炭燃燒源,石油泄漏源,生物質(zhì)燃燒源和交通源;4個(gè)污染源的貢獻(xiàn)率分別為:40.9%,23.9%,23.6%和11.5%。此外,本研究試圖估算研究區(qū)50000 km2范圍內(nèi)PAHs的沉降通量,年沉降通量約為107.8 t。
[Abstract]:The river basin, estuarine and offshore system are affected by the land and the ocean, and the system is stored in complex physical and chemical processes. It is an extremely fragile ecosystem. In addition, the development of the society and economy makes the region still face enormous human activity pressure. A large number of pollutants are placed in the region, making the ecosystem and environment in the system affected. Therefore, it is very important and urgent to study the environmental behavior of pollutants in the system. This study takes the Yangtze River Basin - estuarine near sea environment as a typical study area to analyze the occurrence of persistent organic pollutants, polycyclic aromatic hydrocarbons (Polycyclic aromatic hydrocarbons, PAHs) in the system, and reveal the occurrence of the system. The source, distribution and composition of PAHs in the system, the possible influence factors of the PAHs environmental behavior in the system are deeply explored. The concentration range of dissolved phase PAHs (DPAHs) in the surface water body of the Yangtze River Basin is 17.7ng/L to 110 ng/L, with the average value of 42.6ng/L. as a whole, and the PAHs in the basin from upstream to downstream has a obvious cumulative increasing trend. However, the Three Gorges reservoir has obvious low value, which has obvious regulating effect on the DPAHs of the basin. This may be due to the water storage function of the Three Gorges reservoir has a certain dilute effect on the PAHs. The main body of the basin is low ring PAHs (2-3 ring), and its content is about the 67%. source of the total DPAHs content in the water body. There are four main sources of PAHs: biomass fuel and coal combustion mixing source, petroleum substance leakage source, traffic mixing source (diesel and gasoline engine) and coke source, and the contribution rate of each pollution source is 40.1%, 19.6%, 17.5% and 22.8%. in the middle and lower reaches of the Yangtze River Basin, the concentration distribution of suspended particulate phase PAHs (PPAHs) is 595.91 ng/g - 2 473.74ng/g (dry weight), the average concentration is about 1369.92ng/g. and two lakes (Dongting Lake and Poyang Lake) with high concentration. The concentration of PPAHs also increases gradually from two lakes. The two lakes have their own catchment function, and the basin all belong to the region of rapid economic development. Because of this, they have a certain converging function to PAHs. The downstream reaches (from nine). The PPAHs content in the water body of the river station to Changshu station shows a more obvious cumulative effect, especially at the ZhenJiang Railway Station, and the PPAHs concentration observed at the station in Changshu is obviously lower than that of ZhenJiang Railway Station as well as the influence of the estuarine tidal current in the estuary area. The middle and lower reaches of PPAHs have a certain dilution effect. The main PPAHs in the middle and lower reaches of the river is mainly high molecular weight (4-6 ring), occupying more than 84% of the total amount of PAHs. The total concentration of PAHs in the surface sediments of the Yangtze Estuary and its adjacent sea area is between 26.6-621.6 ng/g (dry weight). The average concentration is about 158.2ng/g. and PAHs in space distribution. It can be divided into two parts: the Yangtze Estuary region and the Zhejiang coastal waters of the southern Hangzhou Bay, the high concentration area appears in the east of the Zhoushan archipelago outside the Hangzhou Bay. The concentration range of PAHs in the surface sediments of the Yangtze Estuary is 27.2-400.9ng/g, with an average concentration of about 137.7ng/g; and near the near Zhejiang. The concentration of PAHs in the surface sediments of the shore is 27.3-621.6 ng/g, the average concentration is about 175.8 ng/g., and the concentration distribution of PAHs is gradually rising from the north to the south, which is in accordance with the grain size of the sediments in the study area. In addition, the concentration of PAHs also changes gradually from the mouth of the estuary to the sea first and then gradually change. The large trend is likely to be affected by the complex hydrodynamic conditions in the estuarine area. As the sediment of the Yangtze River enters the estuary, the mixture of salt and fresh water and the roof of the tidal current accumulate in the estuarine area. In addition, a large number of PAHs in the estuarine busy shipping activities also settle in the estuarine area, making the estuarine area PAHs high value area. However, however, The strong power of the estuarine area, especially the Changjiang River fresh water, makes a large number of PAHs to be taken to the far outside of the mouth area. In the process of transportation, the sediment is sorted and accumulated along with the sediments. In the end, a large number of PAHs and fine sediments are accumulated in the muddy area of the Yangtze Estuary. The high concentration of PAHs in the region is high. The high scores in the whole study area are high. The concentration range of PAHs is about 12.9-436.3 ng/g, and the concentration of PAHs in the 30.3%-89%. research area that occupies the total PAHs concentration is similar to the distribution characteristics of the grain size and organic carbon content of the sediments. However, the correlation analysis shows that the correlation between the three is not obvious. This may be due to the adsorption behavior of PAHs. A complex process, sediment granularity and organic carbon have adsorption preferences, and the strong dynamic conditions in the region also make PAHs redistribute. Therefore, complex control factors make the correlation between the three become blurred. The source analysis results show that the research area PAHs mainly comes from the coal combustion source, the oil leakage source, Biomass combustion source and traffic source; the contribution rate of the 4 sources are 40.9%, 23.9%, 23.6% and 11.5%. respectively. This study attempts to estimate the PAHs settlement flux in the range of 50000 km2 in the study area, and the annual settlement flux is about 107.8 t.
【學(xué)位授予單位】：南京大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X592

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本文編號(hào)：1913342