本文選題：光降解 + 氨氮�。� 參考：《北京化工大學》2015年碩士論文

【摘要】：近年來,水體中環(huán)境雌激素污染嚴重,再生水體中低痕量的環(huán)境雌激素具有很強的雌激素效應(yīng),市民的健康受到威脅,然而目前關(guān)于環(huán)境雌激素在水體中的遷移轉(zhuǎn)化研究尚不全面,已有研究主要報道的是在紫外光照下高濃度雌激素的光降解行為,而實際污染的再生水體中雌激素含量在納克級。本課題在前期對再生水體中雌激素分布調(diào)查研究的基礎(chǔ)上,選取了雌酮為研究對象,采用氙燈模擬太陽光研究水體中雌激素E1光化學轉(zhuǎn)化的影響因素,并探討再生水體中E1的轉(zhuǎn)化機理。首先,研究了純水體系中無機離子對雌激素E1光降解的影響。(1)以氙燈為光源的光降解體系中對環(huán)境雌激素E1的降解速率較快,光照20 min后雌激素E1降解率為87%。(2)研究了不同的無機離子對雌激素E1的影響,如NH4+, N03等,結(jié)果表明：NH4-N會抑制雌激素E1的光降解行為,使雌激素El的降解率下降,且水相中隨著NH4-N濃度的增加,雌激素El的降解率降低,雌激素E1的光降解反應(yīng)速率減小,從而在水相中的半衰期增大。(3)NO3-N可以促進水相中雌激素E1的光降解行為,水相中加入一定量NO3-N,E1的降解率相應(yīng)增加,同時El的光降解反應(yīng)速率增大。(4)NH4-N和NO3-N共存的雌激素水相中,NO3-N對雌激素E1的光降解的促進起主導作用,促進其雌激素E1的降解,且隨著水相中NO3-N和NH4-N濃度比增加,E1降解率增加,E1的光降解反應(yīng)速率增大,即E1在水相中的半衰期縮短。其次,研究了高碑店湖表層水基質(zhì)條件下雌激素El的光降解行為。模擬了太陽光光照高碑店湖表層水基質(zhì)下雌激素E1的實驗,隨著湖水水流方向NH4-N的濃度逐漸增加,雌激素El的光降解反應(yīng)速率逐漸減小,因此NH4-N是影響高碑店湖水體中雌激素El降解的重要因素之一最后,為了探討雌激素El在水體中的轉(zhuǎn)化機理,通過紅外光譜儀、電子自旋共振波譜儀、氣相色譜質(zhì)譜聯(lián)用儀等方法對雌激素El光降解過程及產(chǎn)物進行了研究,同時,研究光降解過程中El水溶液的內(nèi)分泌干擾活性變化。(1)通過紅外光譜研究雌激素E1的降解過程發(fā)現(xiàn)：光降解過程中E1的苯環(huán)遭到破壞,1720 cm-1對應(yīng)的C=O鍵特征峰在光照時間為0、10和20 min樣品中的強度逐漸減弱,而2854 cm-1和2925 cm-1對應(yīng)的脂肪碳的C-H鍵特征峰先增強后減弱,可能是因為E1結(jié)構(gòu)中的C-C=O發(fā)生了反應(yīng)生成了C=C-OH,而隨著反應(yīng)的繼續(xù),C=C也被進一步氧化。(2)通過電子自旋共振波譜研究雌激素El的降解過程發(fā)現(xiàn)：模擬太陽光光照雌激素E1水系反應(yīng)中可能產(chǎn)生了羥基自由基(·OH),其可能的途徑為光照雌激素El產(chǎn)生水合電子(eaq-)。發(fā)生一系列反應(yīng)產(chǎn)生了氧化物質(zhì)如(·OH),進而這些氧化物質(zhì)同雌激素El反應(yīng)使其降解。(3)通過氣相色譜質(zhì)譜研究雌激素E1的降解過程發(fā)現(xiàn)：光降解雌激素E1水系過程中,雌激素E1得到明顯的降低,同時對雌激素E1衍生化產(chǎn)物的圖譜與標準圖譜比對研究,結(jié)果表明雌激素E1在光降解中產(chǎn)生了中間產(chǎn)物。同時也可以看出降解過程中的酮基發(fā)生改變生成了碳碳雙鍵,以及苯環(huán)遭到破壞。(4)通過對光降解過程中的E1的雌激素效應(yīng)研究發(fā)現(xiàn)：其一,隨著光照時間的增加,四種水相中的雌激素E1毒性有顯著的降低,光降解過程中沒有產(chǎn)生比E1毒性更強的雌激素化合物；其二,NH4-N對光降解中雌激素E1毒性影響不大；其三,光降解過程中NO3-N的存在使水溶液的內(nèi)分泌干擾活性降低的更快,最終可能使其雌激素礦化為二氧化碳和水。
[Abstract]:In recent years, environmental estrogens are polluted seriously in the water body. The low trace environmental estrogens in the regenerated water body have a strong estrogen effect, and the health of the citizens is threatened. However, the study on the migration and transformation of environmental estrogens in water bodies is not comprehensive. The main report is that the high concentration of estrogen is light under ultraviolet light. On the basis of the investigation of estrogen distribution in the regenerated water body, the estrone is selected as the research object and the influence factors of the photochemical transformation of estrogen E1 in the water body are studied by using xenon lamp to simulate the photochemical transformation of estrogen in the water body, and the transfer of E1 in the regenerated water body is discussed. First, the effect of inorganic ions on the photodegradation of estrogen E1 in pure water system was studied. (1) the degradation rate of environmental estrogen E1 was faster in the photodegradation system with xenon lamp as the light source. The degradation rate of estrogen E1 after 20 min was 87%. (2), and the effects of different inorganic ions on estrogen E1 were studied, such as NH4+, N03 and so on. NH4-N can inhibit the photodegradation behavior of estrogen E1 and decrease the degradation rate of estrogen El, and with the increase of NH4-N concentration, the degradation rate of estrogen El decreases, the rate of the photodegradation reaction of estrogen E1 decreases, and the half-life in the water phase increases. (3) NO3-N can promote the photodegradation behavior of estrogen E1 in the water phase, and the water phase is added to the water phase. In a certain amount of NO3-N, the degradation rate of E1 increased correspondingly and the photodegradation rate of El increased. (4) in the estrogenic water phase of NH4-N and NO3-N, NO3-N played a leading role in promoting the photodegradation of estrogen E1, promoting the degradation of estrogen E1, and the E1 degradation rate increased with the increase of NO3-N and NH4-N concentration in the water phase and the photodegradation reaction of E1. The rate of the half-life of E1 in the water phase is shortened. Secondly, the photodegradation behavior of estrogen El under the surface water matrix of Gaobeidian lake is studied. The experiment of estrogen E1 under the surface water matrix of Gaobeidian lake is simulated by the sun light light. With the concentration of NH4-N in the water direction of lake water increasing gradually, the rate of photodegradation reaction of estrogen El is gradual. As a result, NH4-N is one of the important factors affecting the degradation of estrogen El in the water of Gaobeidian lake. In order to explore the transformation mechanism of estrogen El in water body, the photodegradation process and products of estrogen El are studied by infrared spectrometer, electron spin resonance spectroscopy, gas chromatography-mass spectrometry and so on. Changes in the endocrine disrupting activity of El aqueous solution during photodegradation (1) the degradation process of estrogen E1 was studied by infrared spectroscopy. It was found that the benzene ring of E1 was destroyed during the photodegradation, and the characteristic peaks of the C=O key corresponding to the 1720 cm-1 were gradually weakened in the light time of 0,10 and 20 min samples, and the 2854 cm-1 and 2925 cm-1 corresponding fats. The characteristic peak of carbon C-H bond first increased and then weakened, probably because of the reaction of C-C=O in the E1 structure to generate C=C-OH, and with the continuation of the reaction, C=C was further oxidized. (2) the degradation process of estrogen El was studied by the electron spin resonance spectroscopy, and it was found that the simulated sun light illuminated the estrogen E1 water system and the hydroxyl group may produce hydroxyl group. The free radical (OH), its possible pathway is the production of hydrous electrons (eaq-) in the light of estrogen El. A series of reactions produce oxidizing substances such as (. OH), and then these oxidizing substances degrade with estrogen El. (3) the degradation process of estrogen E1 was studied by gas chromatography mass spectrometry. E1 was significantly reduced. At the same time, compared with the standard atlas of the estrogen E1 derivatives, the results showed that the estrogen E1 produced intermediate products in the photodegradation. At the same time, it can be seen that the change of the ketone in the degradation process generated carbon carbon double bonds and the benzene ring was destroyed. (4) through the E1 degradation process, the E1 The study of estrogen effect found that: first, with the increase of light time, the toxicity of estrogen E1 in the four water phases decreased significantly, and the estrogen compounds with stronger toxicity than E1 were not produced in the photodegradation process; secondly, the toxicity of NH4-N to the photodegradation of estrogen E1 was not significant; and third, the presence of NO3-N in the process of photodegradation made water. The endocrine disrupting activity of the solution decreases faster, which may eventually lead to the mineralization of its estrogen into carbon dioxide and water.
【學位授予單位】：北京化工大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X52

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