發(fā)布時間：2018-06-24 03:49

  本文選題：雙酚A + 介孔材料��； 參考：《北京理工大學》2015年碩士論文

【摘要】：分子印跡聚合物具有選擇性高、穩(wěn)定性好、抗惡劣環(huán)境能力強等特點,廣泛應用于分離分析、固相萃取、傳感器、藥物檢測等領域。一般方法制得的印跡聚合物結合位點和印跡空穴嵌入較深,吸附動力學時間長,而介孔硅材料結構堅硬,具有比表面積大、空隙容積高、熱穩(wěn)定性好、孔徑大小可調、易功能化的特點,非常適合作為印跡基質以形成表面印跡位點,可以解決傳統(tǒng)分子印跡方法存在的一些不足。本文綜述了分子印跡聚合物的合成方法并分析了各種方法存在的優(yōu)缺點以及硅基印跡基體的發(fā)展過程。介紹了介孔材料MCM-41和SBA-15的合成方法、表征方法及應用,提出了論文的選題依據,研究意義及研究內容。通過優(yōu)化合成條件制備了兩種不同的介孔材料MCM-41和SBA-15作為分子印跡基體,其中MCM-41以十六烷基三甲基溴化銨作為模板劑,在弱堿性環(huán)境中,以正硅酸乙酯為硅源,加入乙醇,氨水調節(jié)pH,經過水熱老化的過程制得。SBA-15的合成以P123三嵌段共聚物作為模板劑,以正硅酸乙酯作為硅源,在酸性條件下通過水熱合成的方法制得,兩種介孔材料都通過高溫煅燒的方法去除模板劑。對介孔材料分別進行了紅外光譜、X射線衍射、SEM表征,然后通過對介孔材料進行氨基化修飾使其能夠形成與模板分子結合的位點,再與模板分子結合制備分子印跡介孔有機硅材料,并通過對兩種不同基體制備的印跡材料進行動力學,吸附等溫線,吸附選擇性,循環(huán)吸附實驗測試。MCM-41基分子印跡介孔硅材料對雙酚A的吸附50 min內達到吸附平衡,吸附選擇性實驗表明MIP的吸附量遠大于NIP的吸附量,并且在有類似物競爭時,對模板分子具有特異性吸附性能。循環(huán)吸附實驗經四次洗脫-吸附-洗脫后吸附量為原來的60%左右,有一定的循環(huán)利用性。SBA-15基分子印跡介孔硅材料的吸附平衡約20 min即可達到吸附平衡,與傳統(tǒng)的分子印跡聚合物相比速率有了較大的提高,對模板分子的吸附有較高的選擇性。四次洗脫-吸附-洗脫后吸附量為原來的50%左右,也保持了一定的循環(huán)使用性。SBA-15基印跡介孔硅材料對實際樣品的應用具有潛在的價值。比較了兩種不同的介孔基印跡聚合物的吸附性能,對印跡聚合物的吸附動力學,吸附等溫線,吸附選擇性以及循環(huán)利用率進行了比較。SBA-15基印跡聚合物的吸附速率和吸附量都遠遠大于MCM-41基印跡聚合物,循環(huán)利用率略低于MCM-41基印跡聚合物。這與基體自身的孔結構有很大的關聯(lián)。使用SBA-15-MIP對水樣品進行雙酚A加標回收實驗,實驗結果對雙酚A的加標回收率在92.8%~99%%之間,結果表明SBA-15-MIP對樣品中雙酚的富集有效。制備的SBA-15基印跡聚合物對雙酚A的吸附在20 min以內達到吸附平衡,較快的吸附速率以及較高的吸附量使得SBA-15基印跡聚合物在雙酚A的富集方面具有較好的實際應用價值。
[Abstract]:Molecularly imprinted polymers (MIPs) are widely used in separation and analysis, solid phase extraction, sensors, drug detection and so on. The imprinted polymer has deep binding sites and imprinted holes, and the adsorption kinetics is long. The mesoporous silicon materials have hard structure, large specific surface area, high void volume, good thermal stability and adjustable pore size. The feature of easy functionalization is very suitable as imprinting substrate to form surface imprinting sites, which can solve some shortcomings of traditional molecular imprinting methods. In this paper, the synthetic methods of molecularly imprinted polymers are reviewed, and the advantages and disadvantages of these methods and the development of silicon-based imprinted matrix are analyzed. The synthesis, characterization and application of mesoporous materials MCM-41 and SBA-15 were introduced. Two kinds of mesoporous materials MCM-41 and SBA-15 were prepared by optimizing the synthesis conditions. MCM-41 used cetyltrimethylammonium bromide as template, ethyl orthosilicate as silicon source, and ethanol was added into MCM-41. In the process of hydrothermal aging, the synthesis of .SBA-15 was prepared by adjusting pH with ammonia water, using P123 triblock copolymers as template and ethyl orthosilicate as silicon source, and was synthesized by hydrothermal method under acidic conditions. Both mesoporous materials were calcined at high temperature to remove the template. The mesoporous materials were characterized by FTIR X-ray diffraction (XRD) SEM, and then modified by amination of mesoporous materials to form sites binding to template molecules. Then the molecular imprinted mesoporous organosilicon materials were prepared by binding with template molecules. The adsorption isotherms and selectivity of the imprinted materials prepared by two different substrates were carried out. The adsorption equilibrium of BPA on MCM-41 based molecularly imprinted mesoporous silicon material was observed in 50 min. The adsorption selectivity experiment showed that the adsorption capacity of MIP was much larger than that of nip, and when there was competition between MCM-41 and MCM-41, the adsorption capacity of MIP was much higher than that of nip. The template molecules have specific adsorption properties. After four times of elution, the adsorption capacity was about 60%, and the adsorption equilibrium of molecular imprinted mesoporous silicon based on SBA-15 was about 20 min. Compared with the traditional molecularly imprinted polymers, the adsorption rate of the template molecules is higher than that of the traditional imprinted polymers. The adsorption capacity of four elution adsorption-elution is about 50%, and the reusability of SBA-15 based imprinted mesoporous silicon material has potential value for the application of practical samples. The adsorption properties, adsorption kinetics and adsorption isotherm of two different mesoporous imprinted polymers were compared. The adsorption rate and adsorption capacity of SBA-15 group imprinted polymer were much higher than that of MCM-41 group imprinted polymer, and the cyclic utilization ratio was slightly lower than that of MCM-41 group imprinted polymer. This is closely related to the pore structure of the matrix itself. SBA-15-MIP was used for the recovery of bisphenol A in water samples. The results showed that the recoveries of bisphenol A were between 92.8% and 99%. The results showed that SBA-15-MIP was effective in the enrichment of bisphenol in water samples. The adsorption equilibrium of SBA-15-group imprinted polymer for bisphenol A was achieved within 20 min. The higher adsorption rate and higher adsorption amount made SBA-15-base imprinted polymer have good practical application value in the enrichment of bisphenol A.
【學位授予單位】：北京理工大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：O631.3;TB383.4

【參考文獻】

相關期刊論文 前2條

1 賈雪平,楊春;酸性條件下合成純硅六方介孔分子篩的條件探索[J];南京師大學報(自然科學版);2001年01期

2 蘇立強;周磊;翟明，

本文編號：2059874