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  本文選題：有機功能化介孔材料 + click反應��； 參考：《大連理工大學》2015年碩士論文

【摘要】：有機基團修飾的介孔氧化硅材料在許多領域表現(xiàn)出潛在的應用價值,包括催化、吸附、藥物傳遞、環(huán)境保護等。由于具有高的比表面積、大而可調(diào)的孔徑、多樣的孔結構,功能化介孔材料是一種很好的去除水體中污染物的吸附劑。通過有機基團的引入,可以強化介孔材料與吸附質(zhì)之間的作用力,例如靜電作用、親/疏水性、π-π鍵以及絡合作用等,從而增強介孔材料的吸附性能。抗生素類藥物進入水環(huán)境后,通過傳統(tǒng)水處理技術難以去除,是一種新興的環(huán)境污染物。圍繞有機功能化的介孔材料合成及吸附去除抗生素污染物的問題,本論文開展了以下研究：共縮聚法合成的疊氮基功能化的介孔SBA-15材料(N3-SBA-15)作為反應的原料,通過click反應將有機基團引入到介孔材料中,結果表明反應高效、產(chǎn)率高。同時用傳統(tǒng)的共縮聚法和后嫁接法合成SBA-15類功能化材料,三種合成方法得到的材料具有相似的官能團。所有材料用于抗生素吸附實驗,結果顯示相似的官能團具有相似的吸附趨勢。但通過click反應制備有機基團功能化介孔材料更加方便、快速并且對材料結構影響較小。由此證明click反應修飾介孔材料的新應用：可以用來迅速篩選吸附抗生素功能基團。上述研究表明介孔材料中引入有機基團,增加材料的疏水性可以提高材料對抗生素的吸附性能。提高材料的疏水性除了可以在材料表面引入有機基團,還可以在材料的表面和骨架中同時引入有機基團。因此,我們進一步合成了骨架中含有乙烷功能團,表面可以通過click反應修飾不同功能團的疊氮基功能化的周期性介孔有機硅材料(PMOs).實驗顯示click反應同樣快速、高產(chǎn)率。此外,修飾后的PMOs比單純疊氮功能化PMOs對抗生素(鹽酸環(huán)丙沙星)的吸附容量明顯提高(241μg/g)。研究表明,click反應可以在PMOs材料中引入多種官能團,環(huán)境應用潛力巨大。為了研究吸附劑與吸附質(zhì)之間的作用力對吸附效果的影響,又做了如下實驗。用共縮聚法合成SBA-15和SH-SBA-15、進而合成SO3H-SBA-15。三種材料做氟喹諾酮類抗生素吸附實驗,結果證明SO3H-SBA-15有突出的吸附性能。通常我們認為吸附劑的疏水性對吸附的影響會強于它們與吸附質(zhì)之間的靜電作用力的影響。但是經(jīng)過實驗以及材料結構分析,對這一現(xiàn)象的推斷是,SO3H-SBA-15與抗生素分子間存在的靜電吸引作用比親／疏水作用更有利于吸附的進行。此外,SO3H-SBA-15在重復利用三次后吸附性能仍然沒有明顯降低,可以說是一種非常有潛力的吸附劑。
[Abstract]:Organic group modified mesoporous silica materials have shown potential applications in many fields, including catalysis, adsorption, drug delivery, environmental protection and so on. Because of its high specific surface area, large and adjustable pore size and diverse pore structure, functionalized mesoporous material is a good adsorbent for removing pollutants in water. The interaction between mesoporous materials and adsorbents, such as electrostatic interaction, hydrophobicity, 蟺-蟺 bond and complexation, can be strengthened by the introduction of organic groups, thus enhancing the adsorption properties of mesoporous materials. After antibiotics enter the water environment, it is difficult to remove by traditional water treatment technology, so it is a new environmental pollutant. In this paper, the synthesis of organic functionalized mesoporous materials and the removal of antibiotic pollutants by adsorption have been studied as follows: the azido-functionalized mesoporous SBA-15 materials (N3-SBA-15) synthesized by co-condensation were used as raw materials for the reaction. The organic groups were introduced into mesoporous materials by click reaction. The results showed that the reaction was efficient and the yield was high. At the same time, the SBA-15 functional materials were synthesized by the traditional co-condensation and post-grafting methods. The materials obtained by the three methods have similar functional groups. All the materials were used in antibiotic adsorption experiments. The results showed that the similar functional groups had similar adsorption trend. However, the preparation of organic group functionalized mesoporous materials by click reaction is more convenient, rapid and has little effect on the structure of the materials. The new application of click reaction modified mesoporous materials can be used to quickly screen functional groups of adsorbed antibiotics. The results show that the addition of organic groups and the increase of hydrophobicity of mesoporous materials can improve the adsorption properties of antibiotics. To improve the hydrophobicity of the material, not only organic groups can be introduced on the surface of the material, but also organic groups can be introduced into the surface and skeleton of the material at the same time. Therefore, we further synthesized the ethane functional group in the skeleton. The surface can be modified by click reaction. The periodic mesoporous organosilicon materials with different functional groups can be modified by click reaction. The experiment showed that click reaction was also fast and high yield. In addition, the adsorption capacity of modified PMOs for antibiotics (ciprofloxacin hydrochloride) was significantly higher than that of azido-functionalized PMOs. The results show that the click reaction can introduce a variety of functional groups into PMOs materials and has great potential for environmental application. In order to study the effect of the force between adsorbent and adsorbate on the adsorption effect, the following experiments have been done. SBA-15 and SH-SBA-15 were synthesized by co-condensation, and then SO3H-SBA-15 was synthesized. The adsorption experiments of fluoroquinolones by three kinds of materials show that SO3H-SBA-15 has outstanding adsorption properties. It is generally considered that the hydrophobicity of adsorbents has a stronger effect on the adsorption than the electrostatic force between them and the adsorbates. However, it is inferred that the electrostatic attraction between SO3H-SBA-15 and antibiotic molecules is more favorable to the adsorption than the hydrophilic / hydrophobic interaction. In addition, the adsorption properties of SO3H-SBA-15 were not significantly decreased after three times of reuse, which can be said to be a very potential adsorbent.
【學位授予單位】：大連理工大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：X52;O647.3

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2 吳s，

本文編號：1913157