【摘要】：鄰苯二甲酸醋類(Phthalicacidesters, PAEs)塑化劑已被廣泛用于各行各業(yè),其環(huán)境風(fēng)險已引起人們高度關(guān)注。環(huán)境中PAEs的內(nèi)分泌干擾效應(yīng)及其降解技術(shù)等為目前專家學(xué)者研究的熱點,但其降解機理研究還較為薄弱。隨著PAEs不斷進入水體環(huán)境,傳統(tǒng)工藝很難將其去除。為減少其潛在風(fēng)險,深入開展水溶液中PAEs降解技術(shù)探索及機理研究顯得非常重要。論文采用紫外光和過硫酸氫鉀(Potassiumperoxymonosulfate,PMS)聯(lián)用以及臭氧氧化的方法,對水體中的鄰苯二甲酸異辛酯(Di(2-ethylhexyl)Phthalate,DEHP)降解效果及機理進行探討。主要成果有:(1) UV/PMS體系降解DEHP的影響因素研究研究考察了 PMS、DEHP濃度、溫度、pH值、環(huán)境中集中常見離子和腐殖酸對DEHP降解速率的影響。結(jié)果表明,①PMS與DEHP配比越高,降解速率常數(shù)越高,但DEHP濃度過高時會抑制反應(yīng)速率;②加熱能加快降解速率,并且是UV/PMS體系中一個重要的影響因素;③在不同pH條件下,酸性條件更適合UV/PMS降解DEHP;④環(huán)境中常見的Fe~(2+)、Co~(2+)、NO3-、HCO3-和腐殖酸對UV/PMS降解DEHP也有影響,除了腐殖酸對反應(yīng)有抑制作用,其他離子都能夠加快降解速率。(2)臭氧降解水中DEHP的影響因素研究研究考察了溫度、pH值對降解速率的影響,結(jié)果表明,①溫度升高能夠加速臭氧降解DEHP的速率;②在pH為11時,速率常數(shù)kapp達到最高值0.011 min-1,即堿性條件更適合臭氧降解DEHP。(3) DEHP降解過程機制及機理研究研究首先對DEHP降解過程中的中間產(chǎn)物進行鑒別,確定其質(zhì)荷比,然后高斯計算,推測DEHP的降解機理。結(jié)果表明,①UV/PMS降解DEHP過程中,共存在7個中間產(chǎn)物,3種降解路徑,UV/PMS通過HO-自由基攻擊和直接氧化結(jié)合的過程,在HO-和SO_4~(·-)共同作用下,HO-會加成在DEHP分子的苯環(huán)上。②臭氧降解DEHP的過程中,存在4個中間產(chǎn)物,2種降解路徑;其主要降解機理也是通過自由基攻擊DEHP和直接氧化的兩種方式的結(jié)合,但在臭氧體系中,只有HO'攻擊DEHP分子上的苯環(huán),沒有發(fā)生加成反應(yīng)。
[Abstract]:(Phthalicacidesters, PAEs) plasticizer of phthalic acid vinegar has been widely used in various industries, and its environmental risk has been highly concerned. The endocrine disrupting effect and degradation technology of PAEs in the environment are the focus of experts and scholars at present, but the study of degradation mechanism of PAEs is still relatively weak. With the continuous entry of PAEs into the water environment, it is difficult to remove it by traditional technology. In order to reduce the potential risk, it is very important to explore the technology and mechanism of PAEs degradation in aqueous solution. The degradation effect and mechanism of iso-octyl phthalate (Di (2-ethylhexyl) Phthalate,DEHP in water were studied by UV light, potassium persulfate (Potassiumperoxymonosulfate,PMS) and ozone oxidation. The main results are as follows: (1) the effects of concentration of PMS,DEHP, temperature, pH value, concentration of common ions and humic acid on the degradation rate of DEHP in UV/PMS system were investigated. The results show that the higher the ratio of 1PMS to DEHP is, the higher the degradation rate constant is, but the higher the concentration of DEHP is, the higher the reaction rate will be; (2) heating can accelerate the degradation rate, and it is an important factor in UV/PMS system. Acid conditions were more suitable for UV/PMS degradation of Fe~ (2), Co~ (2), NO3-,HCO3- and humic acid in DEHP;4 environment, and also had effect on UV/PMS degradation of DEHP, except humic acid had inhibitory effect on the reaction. Other ions were able to accelerate the degradation rate. (2) the factors affecting the degradation of DEHP in water by ozone were investigated. The results showed that the increase of temperature could accelerate the degradation rate of DEHP by ozone, and the degradation rate of DEHP by ozone was 11:00 at pH. Study on Mechanism and Mechanism of ozonation of DEHP. (3) DEHP degradation process; first, the intermediate products in the degradation process of DEHP were identified, the mass charge ratio was determined, and then Gao Si calculated. The degradation mechanism of DEHP was inferred. The results showed that there were 7 intermediate products and 3 degradation pathways in the process of DEHP degradation by 1UV/PMS. UV/PMS was attacked by HO- radical and directly oxidized. Under the combined action of HO- and SO_4~ (-), HO- was added to the benzene ring of DEHP molecule, and there were 4 intermediate products and 2 degradation pathways in the process of degradation of DEHP by ozone. The main degradation mechanism is the combination of free radical attack on DEHP and direct oxidation, but in ozone system, only HO' attacks benzene ring on DEHP molecule, and no addition reaction occurs.
【學(xué)位授予單位】：常州大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：X703

【參考文獻】

相關(guān)期刊論文 前10條

1 嚴佳麗;陳湖星;楊楊;張凱;王麗;熊麗;耿輝;劉德立;;一株高效DEHP降解菌的分離、鑒定及其降解特性[J];微生物學(xué)通報;2014年08期

2 石巖;辛言君;高孟春;;WO_3/TNAs光電極光催化降解水中DMP的性能研究[J];水處理技術(shù);2014年06期

3 劉靜;李亞茹;王杰;陳凱凱;;高級催化氧化法去除水中鄰苯二甲酸酯的研究進展[J];生態(tài)環(huán)境學(xué)報;2014年05期

4 王繼鵬;楊彥;李定龍;;水環(huán)境中DEHP污染現(xiàn)狀及其去除的研究進展[J];化工進展;2014年02期

5 葉婷;康美;黃乾生;董四君;;鄰苯二甲酸二(2-乙基己)酯(DEHP)和鄰苯二甲酸單乙基己基酯(MEHP)長期暴露對海洋青溕(Oryzias melastigma)內(nèi)分泌干擾效應(yīng)的評價[J];生態(tài)毒理學(xué)報;2014年02期

6 劉明華;;塑化劑的危害與預(yù)防分析[J];綠色科技;2013年04期

7 吳維光;史海霞;韓建秋;葛紅雨;;鄰苯二甲酸二乙基己酯在體外對大鼠卵巢顆粒細胞凋亡Caspase通路的影響[J];環(huán)境衛(wèi)生學(xué)雜志;2012年04期

8 譚鎮(zhèn);李傳紅;莫測輝;;惠州市農(nóng)業(yè)土壤中鄰苯二甲酸酯(PAEs)含量的分布特征[J];環(huán)境科學(xué)與管理;2012年05期

9 朱媛媛;田靖;景立新;吳國平;魏復(fù)盛;;不同城市功能區(qū)土壤中酞酸酯污染特征[J];環(huán)境科學(xué)與技術(shù);2012年05期

10 陳永山;駱永明;章海波;宋靜;;設(shè)施菜地土壤酞酸酯污染的初步研究[J];土壤學(xué)報;2011年03期

相關(guān)博士學(xué)位論文 前2條

1 溫志丹;人工濕地基質(zhì)蛭石及其生物膜對鄰苯二甲酸酯的去除及機理[D];哈爾濱工業(yè)大學(xué);2014年

2 王鑫宏;DBP/DEHP單一及與Pb復(fù)合污染對土壤微生物量碳及土壤酶的影響研究[D];東北師范大學(xué);2010年

相關(guān)碩士學(xué)位論文 前2條

1 王麗霞;保護地鄰苯二甲酸酯污染的研究[D];山東農(nóng)業(yè)大學(xué);2007年

2 靳秋梅;鄰苯二甲酸酯類化合物的擬雌激素活性及對小鼠卵巢功能的影響[D];天津醫(yī)科大學(xué);2005年

，

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