本文關(guān)鍵詞：遼河口葦田濕地PAHs分布及源解析復(fù)合受體模型研究　出處：《中國(guó)海洋大學(xué)》2015年碩士論文　論文類(lèi)型：學(xué)位論文

  更多相關(guān)文章： 多環(huán)芳烴 分布 來(lái)源解析 毒性解析 復(fù)合模型

【摘要】：持久性有機(jī)污染物,因具有持久性、生物毒性、生物富集性、遠(yuǎn)距離遷移性及三致作用(致畸、致癌、致突變)等,成為近年來(lái)世界關(guān)注的焦點(diǎn),研究人員對(duì)其開(kāi)展了大量的研究。本文利用GC/MS測(cè)定了遼河口葦田濕地土壤中16種優(yōu)控PAHs的含量,闡述了PAHs在土壤中的分布情況,討論了土壤中PAHs分布的影響因素,研究應(yīng)用正定矩陣因子分解模型(PMF)、Unmix和化學(xué)質(zhì)量平衡模型(CMB)三種單一模型及Unmix-CMB復(fù)合受體模型解析土壤中PAHs的來(lái)源,并將模型進(jìn)一步與毒性當(dāng)量(TEQ)結(jié)合以定量地估算了PAHs污染來(lái)源的毒性貢獻(xiàn)。該研究對(duì)于從源頭對(duì)濕地土壤中PAHs進(jìn)行有效地控制具有重要的意義。濕地土壤中PAHs含量范圍為235-374 ng/g,平均值為287 ng/g,處于輕微污染水平。PAHs的含量尤其是低環(huán)PAHs分布更容易受到土壤有機(jī)碳的影響,土壤粘粒含量對(duì)PAHs濃度的分布也有一定關(guān)系,而陽(yáng)離子交換量則主要對(duì)中高環(huán)PAHs的分布有一定影響。在土壤不同水穩(wěn)性團(tuán)聚體中PAHs的分布中,PAHs含量隨著團(tuán)聚體粒徑的減小而減少,土壤中較大粒徑的團(tuán)聚體對(duì)低分子量PAHs的吸附相對(duì)較強(qiáng)。利用高低分子量比值及同分異構(gòu)體比值法初步推斷,葦田濕地土壤中PAHs的來(lái)源主要有石油產(chǎn)品燃燒和生物質(zhì)燃燒等燃燒源以及石油的泄露等。進(jìn)一步對(duì)土壤中PAHs進(jìn)行定量源解析,PMF模型解析結(jié)果顯示,石油源(31%)、汽油發(fā)動(dòng)機(jī)排放(26%)和柴油發(fā)動(dòng)機(jī)排放(23%)和生物質(zhì)燃燒(20%)為土壤中PAHs的主要來(lái)源；Unmix模型解析結(jié)果表明,石油源的貢獻(xiàn)最大,達(dá)到了43%,汽油機(jī)和柴油機(jī)排放源的貢獻(xiàn)率為35%,生物質(zhì)燃燒也有一定貢獻(xiàn),貢獻(xiàn)率為22%；CMB模型源解析結(jié)果表明,汽油發(fā)動(dòng)機(jī)排放(29%)與柴油發(fā)動(dòng)機(jī)排放(28%)的貢獻(xiàn)最大；生物質(zhì)燃燒和石油類(lèi)產(chǎn)品的輸入對(duì)遼河口葦田濕地土壤中PAHs也有較高貢獻(xiàn),貢獻(xiàn)率分別為21%和22%；這些污染源跟葦田濕地附近的人類(lèi)活動(dòng)諸如交通排放、燒荒和油田開(kāi)采等有密不可分的關(guān)系。本文對(duì)PMF、Unmix和CMB三種模型的解析結(jié)果進(jìn)行了對(duì)比,結(jié)果顯示,三種模型各自解析得到的PAHs模擬值與實(shí)測(cè)值的擬合均表現(xiàn)良好,CMB模型比PMF和Unmix的擬合優(yōu)度稍高,但其誤差百分?jǐn)?shù)絕對(duì)值普遍比PMF和Unmix大,PMF和Unmix模型得到的模擬值也非常接近；CMB模型對(duì)土壤中PAHs來(lái)源貢獻(xiàn)存在低估的問(wèn)題：由于共線性問(wèn)題的存在,Unmix將汽油機(jī)和柴油機(jī)排放源作為一個(gè)因子提取出來(lái)；三種模型解析出石油源、柴油機(jī)和汽油機(jī)排放源在貢獻(xiàn)率上存在一定差異,而生物質(zhì)燃燒源的貢獻(xiàn)率差別不大,這可能與模型自身的算法及參數(shù)的選擇等有較大關(guān)系。為了解決Unmix模型解析過(guò)程中的共線性問(wèn)題,本文進(jìn)一步構(gòu)建了Unmix-CMB復(fù)合模型,其解析結(jié)果顯示,PAHs的主要來(lái)源依次為石油源(43%)、汽油發(fā)動(dòng)機(jī)排放(23%)生物質(zhì)燃燒(22%)和柴油發(fā)動(dòng)機(jī)排放(12%)。為了解不同來(lái)源的毒性效應(yīng),本文將上述受體模型與毒性當(dāng)量(TEQ)結(jié)合起來(lái),PMF-TEQ、Unmix-TEQ、 CMB-TEQ及Unmix-CMB-TEQ的毒性解析結(jié)果表明,汽油機(jī)和柴油機(jī)排放源呈現(xiàn)出最高的毒性貢獻(xiàn),貢獻(xiàn)率分別為64%、61%、96%和63%,表明汽油機(jī)和柴油機(jī)排放具有最大的毒性效應(yīng),PMF-TEQ與Unmix-CMB-TEQ在毒性貢獻(xiàn)率上表現(xiàn)出非常相似的結(jié)果；石油源和生物質(zhì)燃燒在PMF-TEQ、Unmix-TEQ和Unmix-CMB-TEQ的解析結(jié)果中也呈現(xiàn)出一定的毒性貢獻(xiàn),而在CMB-TEQ的結(jié)果中其毒性效應(yīng)基本可以忽略,這些結(jié)果的差異跟模型之間的差異緊密相關(guān)。
[Abstract]:Persistent organic pollutants (persistent organic pollutants), which are persistent, biotoxic, bioaccumulation, long-distance migration and three effects (teratogenicity, carcinogenesis, mutation), have become the focus of world attention in recent years, and researchers have done a lot of research on them. The contents of Liaohe estuary reed wetland soil and the determination of 16 kinds of PAHs control using GC/MS, expounds the distribution of PAHs in soil, the factors affecting the distribution of PAHs in soil is discussed, application of positive matrix factorization model (PMF), Unmix and chemical mass balance model (CMB) three sources the single PAHs model and the Unmix-CMB receptor complex model analysis in the soil, and the model is further and toxic equivalent (TEQ) combined with quantitative estimation of sources of PAHs toxicity contribution. The research is of great significance to the effective control of PAHs in wetland soil from the source. The content of PAHs in wetland soil is 235-374 ng/g, the average value is 287 ng/g, and it is at the level of slight pollution. PAHs content, especially low ring PAHs distribution, is more susceptible to soil organic carbon. Soil clay content also has a certain relationship with PAHs concentration distribution, while cation exchange rate has a certain effect on the distribution of PAHs. In the distribution of PAHs in different soil water stable aggregates, the PAHs content decreases with the decrease of aggregate size. The larger particle aggregates in the soil have relatively strong adsorption for low molecular weight PAHs. Based on the ratio of high and low molecular weight and the ratio of isomer, it is preliminarily deduced that the sources of PAHs in reed wetland soil are mainly petroleum products combustion and biomass burning and oil leakage. Further quantitative source apportionment of PAHs in soil, the analytical results of PMF model shows that the source of oil (31%), gasoline engine emissions of diesel engine emissions (26%) and (23%) and biomass burning (20%) as the main source of PAHs in soil; analytical results of Unmix model showed that the oil source contribution and reached 43% gasoline engine and diesel engine, emission contribution rate is 35%, biomass burning has certain contribution, contribution rate was 22%; CMB model source analysis results show that the engine exhaust emission of diesel engine (29%) and (28%) the largest contribution; biomass combustion and input of petroleum products also have a higher contribution to PAHs Liaohe estuary reed wetland soil, the contribution rate were 21% and 22%; the pollution source with reed wetland near human activities such as traffic emission, burning and oil etc. are closely related. The analysis of PMF, Unmix and CMB results of the three models were compared. The results show that the simulated three models each analytic PAHs values fit with measured values showed good, CMB model is better than PMF and Unmix goodness of fit is slightly higher, but the percentage error absolute value generally than PMF and Unmix that value is very close to the simulated PMF and Unmix model; CMB model underestimated problem of sources of PAHs in soil contribution: owing to collinearity problems, Unmix gasoline engine and diesel engine emission sources as a factor extracted; three model solution precipitation oil source, diesel engine and gasoline engine emissions there are some differences in the contribution rate, and biomass burning source contribution rate is not very different, it may have a greater relationship and its algorithm parameters and model selection. In order to solve the collinearity problem in the process of Unmix model resolution, the Unmix-CMB composite model is further constructed. The analysis results show that the main sources of PAHs are oil source (43%), gasoline engine emission (23%), biomass combustion (22%) and diesel engine exhaust (12%). In order to understand the toxic effects of different sources, the receptor model and toxic equivalent (TEQ) combined with the analysis of PMF-TEQ, Unmix-TEQ, toxicity of CMB-TEQ and Unmix-CMB-TEQ showed that the gasoline engine and diesel engine emission sources showing the highest toxicity contribution, the contribution rate of 64% and 61% respectively, 96% and 63%, showed that emissions has the biggest toxic effect of gasoline engine and diesel engine, PMF-TEQ and Unmix-CMB-TEQ in toxicity contribution rate showed very similar results; in the analytical results of PMF-TEQ, Unmix-TEQ and Unmix-CMB-TEQ also showed certain toxicity with oil source and biomass burning, and result in CMB-TEQ in its toxic effects can be ignored, the difference between these differences are closely related with the model.
【學(xué)位授予單位】：中國(guó)海洋大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類(lèi)號(hào)】：X53;X592

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本文編號(hào)：1339329