【摘要】：糖作為生命體的三大物質(zhì)單元之一,在自然界中在廣泛存在,在生命活動中起著至關(guān)重要的作用。其不僅作為能量物質(zhì)為維持生命體的活動提供能量來源,還作為結(jié)構(gòu)物質(zhì)為細(xì)胞的構(gòu)建提供骨架單元,而且它還有許多不為人所熟知的功能,如免疫反應(yīng)、癌癥的轉(zhuǎn)移、細(xì)胞之間的溝通、病原體引起的傳染病等。糖的檢測和識別對研究生命體的生理過程以及疾病的產(chǎn)生與轉(zhuǎn)移有著重要的意義。因此對生物體內(nèi)各種糖的識別和檢測已經(jīng)成為生命科學(xué)領(lǐng)域的重要內(nèi)容,開發(fā)對糖具有高選擇性和高靈敏度的傳感器有著重要的意義。受自然界中細(xì)胞膜上離子通道的啟發(fā),通過人工合成的方法之制備出具有選擇性、響應(yīng)性和可控性的傳感器件,實現(xiàn)對糖的超靈敏性的檢測,對生物、化學(xué)和材料學(xué)尤其是生物傳感領(lǐng)域都有著十分重要的理論和實際意義。本論文以苯硼酸、二肽單元為識別單元、硫脲為協(xié)同單元、異丙基丙烯酰胺為功能單元,分別合成對糖具有響應(yīng)性的二元和三元智能共聚物,將其修飾到多孔陽極氧化鋁膜的內(nèi)壁,并利用皮安計檢測的方法,構(gòu)建一種新型的智能納米通道,用于多種糖的高靈敏性和高選擇性識別。本論文的工作分為以下三個部分:第一章為綜述部分。對近年來糖的傳感器進行了梳理,分為硼酸類受體和非硼酸類受體的糖傳感器。并對多孔陽極氧化鋁膜在構(gòu)建智能納米通道中的應(yīng)用做了簡要的介紹,進一步介紹了本論文研究的目的和內(nèi)容。第二章將3-丙烯酰硫脲基苯硼酸(ATPBA)與N-異丙基丙烯酰胺(NIPAAm)通過可逆加成-斷裂鏈轉(zhuǎn)移聚合(RAFT)合成的糖響應(yīng)性聚合物PNIPAm-co-PATPBA修飾到PAA膜的內(nèi)壁中,構(gòu)建對糖具有響應(yīng)性的智能納米通道。并對修飾的后的PAA膜進行了掃描電子顯微鏡(SEM)、X射線光電子能譜(XPS)的表征。利用皮安計對構(gòu)建的納米通道對葡萄糖、甘露糖、阿拉伯糖和木糖的響應(yīng)性進行了表征。結(jié)果表明我們構(gòu)建的傳感器對糖具有靈敏的響應(yīng)性和選擇性,當(dāng)糖濃度為10-7 M時,阿拉伯糖、木糖、甘露糖和葡萄糖的電流變化率分別為50%、25%、60%和90%,從而實現(xiàn)對葡萄糖的高靈敏檢測。第三章以具有手性識別作用功能性單元二肽分子(β-Asp-Phe)、響應(yīng)性單元異丙基丙烯酰胺(PNIPAAm)和起調(diào)節(jié)作用的苯基硫脲單體合成的三元共聚物(PNI-β-MAP-diTFP)修飾多孔陽極氧化鋁薄膜,構(gòu)建對糖對映體具有不同響應(yīng)性的智能納米通道,通過皮安計的測量來蘇糖對映體通過納米通道時電流的變化,實現(xiàn)響應(yīng)性的信號的傳遞和放大,用于糖對映體的檢測和識別。
[Abstract]:As one of the three major material units of life, sugar exists widely in nature and plays a vital role in life activities. Not only does it provide a source of energy for sustaining the activity of life, but it also provides a skeleton unit for cell construction as a structural substance, and it also has many unknown functions, such as immune responses, cancer metastasis, Communication between cells, infectious diseases caused by pathogens, etc. The detection and recognition of sugar plays an important role in the study of physiological processes of organisms and the generation and transfer of diseases. Therefore, the recognition and detection of sugar in organisms has become an important content in the field of life science, and it is of great significance to develop sensors with high selectivity and sensitivity to sugar. Inspired by ion channels on cell membranes in nature, selective, responsive and controllable sensing devices were prepared by artificial synthesis to detect the hypersensitivity of sugar. Chemistry and material science, especially biosensor, have important theoretical and practical significance. In this paper, binary and ternary intelligent copolymers were synthesized with phenylboric acid and dipeptide units as recognition units, thiourea as synergistic units and isopropyl acrylamide as functional units, respectively. It was modified into the inner wall of porous anodic alumina membrane, and a novel intelligent nanochannel was constructed by using the method of picoammeter detection, which can be used for the high sensitivity and high selectivity recognition of many kinds of sugar. The work of this thesis is divided into three parts: the first chapter is the summary part. The sugar sensors in recent years are sorted into boric acid receptors and non-boric acid receptors. The application of porous anodic alumina membrane in the construction of smart nanochannels is briefly introduced, and the purpose and content of this thesis are further introduced. In chapter 2, the glycosylresponsive polymer (PNIPAm-co-PATPBA) synthesized by reversible addition-break chain transfer polymerization (RAFT) with 3-acryloyl thiourea-phenylborate (ATPBA) and N-isopropylacrylamide (NIPAAm) was modified into the inner wall of PAA film. An intelligent nanochannel responsive to sugar was constructed. The modified PAA films were characterized by scanning electron microscopy (SEM) (SEM), X-ray photoelectron spectroscopy (XPS). The responsiveness of the constructed nanochannels to glucose, mannose, arabinose and xylose was characterized by a picoammeter. The results showed that the sensor was sensitive and selective to sugar. When sugar concentration was 10-7 M, the current change rates of arabinose, xylose, mannose and glucose were 50% and 90%, respectively. In order to achieve the high sensitivity of glucose detection. In Chapter 3, the chiral recognition of functional unit dipeptide molecules (尾-Asp-Phe), Reactive unit isopropyl acrylamide (PNIPAAm) and a terpolymer (PNI- 尾-MAP-diTFP) synthesized by adjusting phenyl thiourea monomer were used to modify porous anodic alumina film. An intelligent nanochannel with different responsiveness to glucose enantiomers was constructed. The changes of electric current of threonose enantiomers through nanowires were measured by a picoammeter to transmit and amplify responsive signals for detection and recognition of sugar enantiomers.
【學(xué)位授予單位】：武漢理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TB383.1;TP212

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