本文關(guān)鍵詞：環(huán)糊精提取技術(shù)評估土壤PAHs生物有效性的機制與模型　出處：《大連理工大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 環(huán)糊精提取技術(shù) 多環(huán)芳烴 生物有效性 評估模型 生態(tài)風(fēng)險

【摘要】：多環(huán)芳烴(Polycyclic Aromatic Hydrocarbon,PAHs)是一類典型的疏水性有機污染物,廣泛存在于土壤中,且具有致畸、致癌和致突變效應(yīng)。羥丙基-β-環(huán)糊精(Hydroxypropyl-β-cyclodextrin,HPCD)提取技術(shù)是評估污染物生物有效性的技術(shù)之一,主要用于開展HPCD對污染物的生態(tài)風(fēng)險評估。然而由于目前所研究污染物的種類單一,使其忽略了污染物之間的化學(xué)多樣性的影響,進而使得HPCD提取技術(shù)評估污染物生物有效性的機制認(rèn)識不夠完善。本研究采用野外土壤綜合考察HPCD對15種PAHs的包合作用、脫附性能及蚯蚓富集的影響,分別從PAHs環(huán)境賦存、生物效應(yīng)等方面明確PAHs的化學(xué)多樣性及HPCD對土壤中PAHs的提取機制,從而闡明HPCD提取評估土壤中PAHs生物有效性的機制并在此基礎(chǔ)上建立HPCD提取與蚯蚓富集的預(yù)測模型。通過加速溶劑提取技術(shù)測試了31種土壤中15種PAHs的總量。通過雙比值法分析表明高速公路附近土壤的PAHs主要來自化石燃料高溫燃燒,化工廠、焦化廠和農(nóng)田附近PAHs主要來自石油揮發(fā)和煤、木材等燃燒,而港口附近的PAHs主要為復(fù)合污染。通過對土壤中PAHs總量與土壤理化性質(zhì)的相關(guān)性分析可知,土壤中PAHs的總量與土壤有機碳含量、比表面積、土壤粘粒分?jǐn)?shù)和砂粒分?jǐn)?shù)正相關(guān),其關(guān)系式為CPAHs=0.48X1+0.33X2+0.36X5+0.20X7(R2=0.95,n=31)不同種類PAHs的濃度分別與土壤有機碳含量、比表面積、孔容、孔徑、粒級分?jǐn)?shù)和風(fēng)化指數(shù)相關(guān)(R2=0.54～0.94,n=31)。結(jié)果表明,不同種類PAHs的環(huán)境賦存存在差異。通過蚯蚓富集實驗研究了蚯蚓對不同土壤中PAHs的富集能力。結(jié)果表明,PAHs未校正及校正BSAF的平均值分別在0.06±0.04(1nP)～0.18±0.10(Nap)和0.12±0.05(1nP) ～0.35±0.11(Nap)之間。根據(jù)Statistic Package for SOcial Science(SPSS)相關(guān)性分析表明,不同種類PAHs的未校正BSAF與土壤和PAHs的理化性質(zhì)相關(guān),其關(guān)系式為logBSAF=-0.98X3+0.35X5+0.48X8+0.15X9-1.00X11+0.45X15-0.28X16(R2=0.80,n=390),其相關(guān)性因素分別為有機碳含量、分子極化率、粘粒分?jǐn)?shù)、粉粒分?jǐn)?shù)、摩爾體積和生物降解速率,其中土壤有機碳含量和PAHs的分子極化率對BSAF (Biota-Soil Accumulation Factor.的貢獻(xiàn)較大。結(jié)果表明,蚯蚓對PAHs富集能力的差異是PAHs的自身理化性質(zhì)及環(huán)境賦存共同作用的結(jié)果。通過HPCD脫附動力學(xué)實驗及有效態(tài)提取技術(shù)研究了HPCD提取評估土壤中PAHs生物有效性的機制,并在此基礎(chǔ)上建立HPCD提取與蚯蚓富集之間的預(yù)測模型。通過SPSS相關(guān)性分析表明,PAHs的HPCD提取濃度與土壤總量濃度的比值及BSAF二者共同與土壤有機碳含量、生物降解速率、粘粒分?jǐn)?shù)和粉粒分?jǐn)?shù)相關(guān),其中有機碳含量貢獻(xiàn)最大。HPCD提取后土壤理化性質(zhì)的變化與蚯蚓富集過程類似,二者均使土壤中的大顆粒轉(zhuǎn)化為小顆粒且比表面積增大,且反應(yīng)HPCD包合能力的包合常數(shù)與反應(yīng)蚯蚓富集能力的BSAF共同與PAHs分子極化率和摩爾體積相關(guān)。結(jié)果表明,HPCD提取過程能夠模擬蚯蚓在土壤中的富集過程且二者可能具有相關(guān)性。利用SPSS曲線估計建立26種土壤中15種PAHs蚯蚓體內(nèi)濃度與HPCD提取濃度的逐一預(yù)測模型(Cworm=((CHPCD+k)/a)0.5+h)(R2=0.88～0.95,n=26))。將18種土壤中15種PAHs的單個及總量濃度混合,建立蚯蚓體內(nèi)濃度與HPCD提取濃度之間的混合模型,Cworm=((CHPCD+91.58)/0.0049)0.5-136.96(R2=0.96,n=270),并隨機選取4種不同類型的8種土壤對預(yù)測模型進行驗證。結(jié)果表明,通過模型得到的蚯蚓預(yù)測值與實測值之間相關(guān)性很好,關(guān)系式為y=1.21x-0.13(R2=0.93,n=120)。利用26種土壤中15種PAHs的蚯蚓體內(nèi)摩爾總量濃度與HPCD提取摩爾總量濃度之間的關(guān)系建立模型(Cworm=((CHPCD-0.018)/1.48)0.5-0.239)(R2=0.92,n=26))并結(jié)合蚯蚓CBR指標(biāo)可知,當(dāng)蚯蚓體內(nèi)濃度為臨界濃度、假設(shè)性安全水平、無明顯效應(yīng)和半致死濃度時所對應(yīng)的HPCD提取摩爾總量分別為0.11 mmol/kg OC,0.37 mmol/kg OC,69 mmol/kg OC和3735 mmol/kgOC；基于HPCD提取與土壤總量比值的正態(tài)分布函數(shù),提出能夠反映99%的土壤中不同影響水平下PAHs的摩爾總量分別為0.15 mmol/kg OC,0.52 mmol/kg OC,57 mmol/kg OC和5261 mmol/kg OC,從而為土壤中PAHs生態(tài)風(fēng)險指標(biāo)的建立提供參考。
[Abstract]:Polycyclic aromatic hydrocarbons (Polycyclic Aromatic, Hydrocarbon, PAHs) is a kind of typical hydrophobic organic pollutants, exists widely in the soil, and has teratogenic, carcinogenic and mutagenic effect of hydroxypropyl beta cyclodextrin (Hydroxypropyl- beta -cyclodextrin, HPCD) extraction technology is one of effective assessment of pollutants biological technology, mainly used for to carry out the HPCD ecological risk assessment of pollutants. However, due to the research on the type of pollutant is single, to ignore the pollutants between the effects of chemical diversity, which makes the HPCD extraction mechanism of technology assessment of pollutants biological knowledge is not perfect. This research adopts the comprehensive field investigation of soil HPCD of 15 PAHs inclusion effect of removal effect of performance and earthworm enrichment, respectively from the PAHs occurrence, biological effects of specific aspects of PAHs chemical diversity and HPCD extraction machine in soil PAHs In order to clarify the HPCD extraction system, evaluation mechanism of the bioavailability of PAHs in soils and on this basis to establish a prediction model of HPCD extraction and enrichment of earthworm. By 31 15 PAHs soil total test accelerated solvent extraction technology. Through the double ratio method analysis shows that the highway near the soil PAHs mainly comes from the combustion of fossil fuel chemical plant, coking plant, and farmland near PAHs mainly from oil and coal volatile, combustion, and near the port of PAHs is the main compound pollution. Based on the correlation between soil total PAHs and soil physicochemical properties analysis showed that the total content of PAHs in soil and soil organic carbon content, surface area, soil the clay fraction and sand fraction is related to its relationship to CPAHs=0.48X1+0.33X2+0.36X5+0.20X7 (R2=0.95, n=31) concentration of different kinds of PAHs respectively and soil organic carbon content, specific surface area, Kong Rong, Aperture, size fraction and weathering index (R2=0.54 ~ 0.94, n=31). The results show that there are different types of PAHs in environmental differences. Earthworms on PAHs in different types of soil enrichment ability was studied by earthworm enrichment experiments. The results show that the PAHs correction and BSAF mean respectively in 0.06 + 0.04 (1nP 0.18) ~ (Nap) + 0.10 and 0.12 + 0.05 (1nP + 0.11) - 0.35 (Nap). According to the Statistic Package for SOcial between Science (SPSS) correlation analysis showed that the physicochemical properties of the uncorrected BSAF and soil and PAHs different kinds of PAHs, its relationship to logBSAF=-0.98X3+0.35X5+0.48X8+0.15X9-1.00X11+0.45X15-0.28X16 (R2=0.80, n=390) the correlation factors, respectively, organic carbon content, molecular polarizability, clay fraction, particle fraction, molar volume and biodegradation rate, the molecular polarization of soil organic carbon content and the rate of PAHs to BSAF (Biota -Soil Accumulation Factor. great contribution. The results showed that the difference of earthworm enrichment ability to PAHs is PAHs its physicochemical properties and interaction environment occurrence results. Through the HPCD removal and available experimental study on Extraction Kinetics of evaluation mechanism of PAHs bioavailability in soil HPCD extraction technology, and on this basis to establish a prediction model HPCD extraction and enrichment of earthworms between. Through the SPSS correlation analysis showed that the ratio of BSAF and HPCD extraction and the concentration of PAHs soil total concentration of two together with the soil organic carbon content, biodegradation rate, clay fraction and particle fraction, which changes with the content of organic carbon.HPCD after extraction of soil physicochemical properties with the earthworm bioaccumulation process is similar, the two are the large soil particles into small particles and the specific surface area increased, and the reaction ability of HPCD inclusion inclusion constant and reaction The enrichment ability of earthworm BSAF and PAHs molecular polarizability and molar volume. The results show that the HPCD extraction process can enrichment process simulation of earthworms in the soil in two and may have correlation. 26 kinds of model estimation by the 15 kinds of soil PAHs concentration and HPCD concentration in earthworm extract by using SPSS curve (Cworm= ((CHPCD+k) /a) 0.5+h (R2=0.88) - 0.95, n=26)). 18 kinds of 15 kinds of PAHs in soil and the total concentration of single hybrid, hybrid model is established between earthworm extraction concentration and HPCD concentration, Cworm= ((CHPCD+91.58) /0.0049) 0.5-136.96 (R2=0.96, n=270), were randomly selected to verify 8 prediction models for 4 different types of soil. The results show that the model obtained by earthworms between predicted and measured values have a good correlation, the relation model is y=1.21x-0.13 (R2=0.93, n=120). The use of 26 kinds of 15 kinds of soil earthworm PAHs A model of the relationship between the total body molar concentration and HPCD molar extraction total concentration (Cworm= ((CHPCD-0.018) /1.48) 0.5-0.239) (R2=0.92, n=26)) combined with earthworm CBR index shows that when the earthworm concentration is the critical concentration, hypothetical safety level, corresponding to no obvious effect and semi lethal concentration of HPCD extraction the total molar were 0.11 mmol/kg OC, 0.37 mmol/kg OC, 69 mmol/kg OC and 3735 mmol/kgOC; normal distribution function of HPCD extraction and the amount of soil is proposed based on the ratio of 99% in soil can reflect the different effects of total level of PAHs Moore were 0.15 mmol/kg OC, 0.52 mmol/kg OC, 57 mmol/kg OC and 5261 mmol/kg OC, so as to provide reference for the establishment of soil PAHs ecological risk index.

【學(xué)位授予單位】：大連理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X825

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本文編號：1420197