【摘要】：化學(xué)發(fā)光法由于其檢測(cè)過(guò)程具有無(wú)背景光干擾且方法靈敏度高的優(yōu)點(diǎn),常被用于分析化學(xué)領(lǐng)域。其中雙(2,4,6-三氯苯基)草酸酯-過(guò)氧化氫體系由于量子產(chǎn)率高、雜質(zhì)干擾小以及可以在接近中性pH條件下進(jìn)行化學(xué)發(fā)光反應(yīng),不僅可以對(duì)小分子進(jìn)行分析檢測(cè),而且也適合對(duì)生物分子進(jìn)行分析檢測(cè)。介孔二氧化硅作為一種納米材料,具有較大的孔容、可調(diào)的孔道結(jié)構(gòu)、表面基團(tuán)易于被修飾以及良好的生物相容性等特點(diǎn),在生物和分析領(lǐng)域應(yīng)用廣泛。氧化石墨烯量子點(diǎn)(GOQDs)不僅保持了GO原有的生物相容性、低毒性等優(yōu)異特點(diǎn),還展現(xiàn)出很強(qiáng)的化學(xué)發(fā)光增敏作用。本文主要基于化學(xué)發(fā)光共振能量轉(zhuǎn)移體系,完成了一些化學(xué)發(fā)光分析檢測(cè)方法的構(gòu)建以及應(yīng)用。具體概述如下:(1)以化學(xué)發(fā)光共振能量轉(zhuǎn)移體系為基礎(chǔ),利用以單鏈DNA作為門(mén)控且用GOQD包裹的介孔二氧化硅合成了一種具有三重信號(hào)放大機(jī)制的生物傳感器,分別采用傅里葉變換紅外光譜儀、紫外-可見(jiàn)分光光度法、Zeta電位等方法進(jìn)行了表征。實(shí)驗(yàn)結(jié)果表明,當(dāng)miRNA-21的濃度在0.005~50 pmol L~(-1)范圍內(nèi),該體系的化學(xué)發(fā)光相對(duì)強(qiáng)度與mi RNA-21的濃度的對(duì)數(shù)存在很好的線(xiàn)性關(guān)系,檢出限為0.002 pmol L~(-1),實(shí)際樣品(人體血清樣品)加標(biāo)回收率為93.6%-108.8%。(2)利用氧化石墨烯量子點(diǎn)(GOQD)的化學(xué)發(fā)光增敏特性,構(gòu)建一種4-硝基苯酚的超靈敏、高選擇性的檢測(cè)方法。實(shí)驗(yàn)結(jié)果表明,當(dāng)4-硝基苯酚的濃度在1.0~300 pmol L~(-1)范圍內(nèi),該體系的化學(xué)發(fā)光相對(duì)強(qiáng)度與4-硝基苯酚的濃度存在很好的線(xiàn)性關(guān)系,檢出限為0.3 pmol L~(-1),實(shí)際樣品(自來(lái)水和湘江水)加標(biāo)回收率為93.4%-107.9%。(3)以化學(xué)發(fā)光共振能量轉(zhuǎn)移體系為基礎(chǔ),結(jié)合氧化石墨烯(GO)的化學(xué)發(fā)光猝滅作用,利用谷胱甘肽(GSH)的還原氧化石墨烯的特性,使化學(xué)發(fā)光恢復(fù),構(gòu)建了一種簡(jiǎn)單、快捷、靈敏的檢測(cè)谷胱甘肽的方法。實(shí)驗(yàn)結(jié)果表明,當(dāng)谷胱甘肽的濃度在0.1~200 nmol L~(-1)范圍內(nèi),該體系的化學(xué)發(fā)光相對(duì)強(qiáng)度與谷胱甘肽的濃度存在很好的線(xiàn)性關(guān)系,檢出限為30 pmol L~(-1),實(shí)際樣品(人體血清樣品)加標(biāo)回收率為93.0%-103.0%。
[Abstract]:Chemiluminescence method is often used in analytical chemistry because of its advantages of no background interference and high sensitivity. The bis (2,4,6-trichlorophenyl) oxalate-hydrogen peroxide system, due to its high quantum yield, low impurity interference and chemiluminescence reaction under near neutral pH conditions, can not only analyze and detect small molecules, It is also suitable for analysis and detection of biomolecules. Mesoporous silica, as a kind of nano-material, has the characteristics of large pore volume, adjustable pore structure, easy modification of surface groups and good biocompatibility. It has been widely used in biological and analytical fields. Graphene oxide quantum dots (GOQDs) not only maintain the original biocompatibility and low toxicity of GO, but also exhibit strong chemiluminescence sensitization. In this paper, based on the chemiluminescence resonance energy transfer system, some chemiluminescence analysis and detection methods have been constructed and applied. The main contents are as follows: (1) based on the chemiluminescence resonance energy transfer system, a biosensor with triple signal amplification mechanism was synthesized by using mesoporous silica coated with GOQD and gated with single strand DNA. Fourier transform infrared spectroscopy, UV-vis spectrophotometry and Zeta potential were used respectively. The experimental results show that there is a good linear relationship between the relative intensity of chemiluminescence and the logarithm of miRNA-21 concentration when the concentration of miRNA-21 is in the range of 0.005 ~ 50 pmol L ~ (- 1), and the detection limit is 0.002 pmol / L ~ (- 1). The standard recovery of the actual sample (human serum sample) was 93.6% ~ 108.8%. (2) the chemiluminescent properties of graphene oxide quantum dot (GOQD) were used to construct a 4-nitrophenol hypersensitivity. A highly selective detection method. The results show that when the concentration of 4-nitrophenol is in the range of 1.0 ~ 300 pmol L ~ (- 1), there is a good linear relationship between the relative intensity of chemiluminescence and the concentration of 4-nitrophenol, and the detection limit is 0.3 pmol / L ~ (- 1). The standard recovery of actual samples (tap water and Xiangjiang water) was 93.4% ~ 107.9%. (3) on the basis of chemiluminescence resonance energy transfer system, combined with the chemiluminescence quenching effect of graphene oxide (GO), Based on the reduction of graphene oxide by glutathione (GSH), a simple, rapid and sensitive method for the determination of glutathione was developed to restore chemiluminescence. The results showed that there was a good linear relationship between the relative intensity of chemiluminescence and the concentration of glutathione in the range of 0.1 脳 200 nmol / L ~ (- 1) of glutathione, and the detection limit was 30 pmol / L ~ (- 1). The standard recovery rate of actual sample (human serum sample) was 93.0% ~ 103.0%.
【學(xué)位授予單位】：湘潭大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類(lèi)號(hào)】：O657.3

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本文編號(hào)：2437154