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

【摘要】：有機(jī)基團(tuán)修飾的介孔氧化硅材料在許多領(lǐng)域表現(xiàn)出潛在的應(yīng)用價(jià)值,包括催化、吸附、藥物傳遞、環(huán)境保護(hù)等。由于具有高的比表面積、大而可調(diào)的孔徑、多樣的孔結(jié)構(gòu),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(jī)基團(tuán)的引入,可以強(qiáng)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(luò)合作用等,從而增強(qiáng)介孔材料的吸附性能�？股仡愃幬镞M(jìn)入水環(huán)境后,通過傳統(tǒng)水處理技術(shù)難以去除,是一種新興的環(huán)境污染物。圍繞有機(jī)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(yīng)的原料,通過click反應(yīng)將有機(jī)基團(tuán)引入到介孔材料中,結(jié)果表明反應(yīng)高效、產(chǎn)率高。同時(shí)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(tuán)。所有材料用于抗生素吸附實(shí)驗(yàn),結(jié)果顯示相似的官能團(tuán)具有相似的吸附趨勢(shì)。但通過click反應(yīng)制備有機(jī)基團(tuán)功能化介孔材料更加方便、快速并且對(duì)材料結(jié)構(gòu)影響較小。由此證明click反應(yīng)修飾介孔材料的新應(yīng)用：可以用來迅速篩選吸附抗生素功能基團(tuán)。上述研究表明介孔材料中引入有機(jī)基團(tuán),增加材料的疏水性可以提高材料對(duì)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(jī)基團(tuán),還可以在材料的表面和骨架中同時(shí)引入有機(jī)基團(tuán)。因此,我們進(jìn)一步合成了骨架中含有乙烷功能團(tuán),表面可以通過click反應(yīng)修飾不同功能團(tuán)的疊氮基功能化的周期性介孔有機(jī)硅材料(PMOs).實(shí)驗(yàn)顯示click反應(yīng)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(duì)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(yīng)可以在PMOs材料中引入多種官能團(tuán),環(huán)境應(yīng)用潛力巨大。為了研究吸附劑與吸附質(zhì)之間的作用力對(duì)吸附效果的影響,又做了如下實(shí)驗(yàn)。用共縮聚法合成SBA-15和SH-SBA-15、進(jìn)而合成SO3H-SBA-15。三種材料做氟喹諾酮類抗生素吸附實(shí)驗(yàn),結(jié)果證明SO3H-SBA-15有突出的吸附性能。通常我們認(rèn)為吸附劑的疏水性對(duì)吸附的影響會(huì)強(qiáng)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(shí)驗(yàn)以及材料結(jié)構(gòu)分析,對(duì)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(jìn)行。此外,SO3H-SBA-15在重復(fù)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(xué)位授予單位】：大連理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X52;O647.3

【共引文獻(xiàn)】

相關(guān)期刊論文 前2條

1 陳一土;郝仕油;;以陰離子表面活性劑合成氨基功能化介孔氧化硅及其Pb~(2+)的去除性能（英文）[J];稀有金屬材料與工程;2012年S3期

2 曾峰;潘真真;張夢(mèng);黃永焯;崔彥娜;徐勤;;有序介孔二氧化硅納米粒的制備及其腫瘤診療應(yīng)用[J];化學(xué)進(jìn)展;2015年10期

相關(guān)博士學(xué)位論文 前1條

1 祖雷;介孔有機(jī)無機(jī)納米復(fù)合顆粒的合成及結(jié)構(gòu)研究[D];延邊大學(xué);2014年

相關(guān)碩士學(xué)位論文 前2條

1 孫佩;一維有機(jī)晶型材料的設(shè)計(jì)合成、表征及催化應(yīng)用研究[D];蘭州大學(xué);2014年

2 吳s，

本文編號(hào)：1913157