本文選題：碳量子點 + 石墨烯　； 參考：《聊城大學(xué)》2016年碩士論文

【摘要】：電致化學(xué)發(fā)光(ECL)是由電化學(xué)反應(yīng)產(chǎn)生的化學(xué)發(fā)光,由于其不需要外加激發(fā)光源,而且背景信號低,線性范圍寬,設(shè)備簡單,現(xiàn)已成為一種應(yīng)用廣泛的具有高靈敏度和高選擇性的檢測方法。ECL免疫傳感器是將電致化學(xué)發(fā)光技術(shù)和免疫技術(shù)的優(yōu)點相結(jié)合而發(fā)展的產(chǎn)物。免疫分析信號增強技術(shù)一直是免疫分析領(lǐng)域研究的一個重要課題,而將抗體與抗原固定在傳感器表面是一個非常重要的步驟,這對于提高傳感器的靈敏度至關(guān)重要。近年來,新型納米材料、信號增強技術(shù)和蛋白質(zhì)固定化技術(shù)在電化學(xué)免疫傳感器檢測腫瘤標(biāo)志物中的應(yīng)用研究頗受關(guān)注。納米技術(shù)與免疫分析方法的結(jié)合為免疫分析的研究與發(fā)展提供了新的思路,特別是復(fù)合納米材料具有獨特的性質(zhì),對發(fā)展高靈敏的免疫傳感器起了非常重要的作用。近年來,新型碳納米材料如碳納米管(CNTs)、石墨烯(Graphene)、碳量子點(CQDs)等由于其獨特的性質(zhì)而被廣泛應(yīng)用于很多領(lǐng)域。石墨稀因具有大的比表面積、機械強度高、化學(xué)穩(wěn)定性高、導(dǎo)熱性突出等優(yōu)點而廣泛應(yīng)用于能量儲存和轉(zhuǎn)換、催化、醫(yī)學(xué)、生物傳感器等方面。碳量子點因具有穩(wěn)定的化學(xué)組成、低毒性、發(fā)光性能優(yōu)良、制備成本低和生物相容性等特點,在生物成像、光電催化、氧化還原、藥物識別等領(lǐng)域具有良好的應(yīng)用前景。本文主要以功能化碳量子點的制備及其在電化學(xué)生物傳感器中的應(yīng)用為主旨,具體開展了以下研究工作:1.碳量子點及含雜碳量子點的制備與表征成功制備了碳量子點(CQDs)及含雜碳量子點,用TEM對其外貌形態(tài)進行了表征,用紫外吸收光譜和熒光光譜對其光學(xué)行為進行了研究,同時還研究了其電化學(xué)發(fā)光行為。結(jié)果顯示,制備的CQDs及含雜CQDs,其顆粒均一,具有可控發(fā)光性,而且電化學(xué)發(fā)光信號穩(wěn)定。另外,還利用CQDs的還原性,成功制備了具有多面體結(jié)構(gòu)的納米金顆粒(AuNPs),這與傳統(tǒng)方法制備的AuNPs是不同的。2.一種基于CQDs的測量癌胚抗原(CEA)的電化學(xué)發(fā)光夾心免疫傳感器成功制備了一種基于CQDs測量CEA的電化學(xué)發(fā)光夾心免疫傳感器。用聚多巴胺和銀納米顆粒的聚合物(PDA-AgNPs)作為平臺固定一抗(Ab1),同時也能夠提高電子傳導(dǎo)速率。CQDs通過氨基固定在聚乙烯亞胺(PEI)功能化的石墨烯氧化物(GO)上,然后將AuNPs固定在CQDs-PEI-GO上后再與二抗(Ab2)鍵合。通過CEA與Ab1和Ab2的結(jié)合,CQDs能夠固定在電極表面而產(chǎn)生電化學(xué)發(fā)光信號。在最佳實驗條件下,該傳感器ECL強度與CEA濃度的對數(shù)呈線性關(guān)系,線性方程為IECL=3380.3+1138.4 lg cCEA/ng mL-1,相關(guān)系數(shù)為R=0.9989,CEA的最低檢出限為1.67 pg mL-1(S/N=3)。該傳感器還成功應(yīng)用于實際樣品中CEA的檢測。該傳感器具有良好的靈敏度、穩(wěn)定性、特異性和重現(xiàn)性,有望應(yīng)用于疾病診斷中。3.一種基于CQDs與聯(lián)吡啶釕(Ru(bpy)32+)共反應(yīng)檢測雙酚A(BPA)的電化學(xué)發(fā)光傳感器成功制備了一種基于CQDs與Ru(bpy)32+共反應(yīng)測定BPA的ECL傳感器。將CQDs固定在聚吡咯功能化的石墨烯氧化物(PPy-GO)上制備了復(fù)合物PPy-GO-CQDs并修飾在電極表面,PPy-GO不僅能夠負載大量CQDs而且能夠加快電極與溶液之間的電子傳輸,進而提高檢測的靈敏度。然后用修飾好的電極在含有Ru(bpy)32+的溶液中,利用BPA對Ru(bpy)32+/CQDs發(fā)光體系的ECL的猝滅作用來檢測BPA。在最佳實驗條件下,該傳感器對BPA檢測的線性范圍為5-1000 nmol mL-1,檢出限為2 nmol mL-1。實驗證明該傳感器具有良好的穩(wěn)定性,較高的靈敏度和更低的檢出限和更寬的線性范圍。4.基于碳量子點(CQDs)做聯(lián)吡啶釕(Ru(bpy)32+)電化學(xué)發(fā)光的共反應(yīng)劑對癌胚抗原(CEA)的高靈敏檢測成功制備了一種基于CQDs與Ru(bpy)32+共反應(yīng)測定CEA的夾心免疫ECL傳感器。將CQDs固定在PEI-GO上,然后選用CQDs-PEI-GO復(fù)合物來固定一抗Ab1。用介孔硅(MSN)負載Ru(bpy)32+和固定AuNPs,其中AuNPs能夠增加電子的傳導(dǎo)進而增大ECL信號。同時,將二抗Ab2固定在MSN上。這里,CQDs作為Ru(bpy)32+發(fā)光的共反應(yīng)劑。在最佳實驗條件下,該傳感器的線性范圍為1 pg·mL-1-1000ng·mL-1,檢出限是0.33 pg mL-1(S/N=3)。該傳感器具有良好的特異性、穩(wěn)定性和重現(xiàn)性。
[Abstract]:Electrochemiluminescence (ECL) is an electrochemiluminescence (chemiluminescence) produced by electrochemical reaction. Because it does not need an excited light source, and the background signal is low, the linear range is wide and the equipment is simple, it has become a widely used detection method with high sensitivity and high selectivity,.ECL immune sensor is the Electrochemiluminescence and immunization technology. The immunoassay signal enhancement technology has been an important subject in the field of immunization analysis, and it is a very important step to immobilized the antibody and antigen on the surface of the sensor, which is very important to improve the sensitivity of the sensor. In recent years, the new nano materials, signal enhancement technology and The application of protein immobilization technology in the detection of tumor markers by electrochemical immunosensor has attracted much attention. The combination of nanotechnology and immunoassay method provides a new idea for the research and development of immunoassay, especially the unique properties of the composite nanomaterials, which are very important for the development of highly sensitive immune sensors. In recent years, new carbon nanomaterials, such as carbon nanotubes (CNTs), graphene (Graphene) and carbon quantum dots (CQDs), have been widely used in many fields because of their unique properties. Graphite thinning has been widely used in energy storage and energy storage because of its large specific surface area, high mechanical strength, high chemical stability, high thermal conductivity and so on. Carbon quantum dots have good application prospects in the fields of bioimaging, photoelectrocatalysis, oxidation-reduction, and drug recognition because of their stable chemical composition, low toxicity, good luminescence, low preparation cost and biocompatibility. This paper mainly focuses on the preparation of functional carbon quantum dots. And its application in electrochemical biosensor is the main purpose. The following research work has been carried out: the preparation and characterization of 1. carbon quantum dots and hetero carbon quantum dots (QDs) have successfully prepared carbon quantum dots (CQDs) and heterocarbon quantum dots. The morphology of them was characterized by TEM, and the optical behavior of them was carried out by UV absorption and fluorescence spectra. At the same time, the electrochemical luminescence behavior was also studied. The results showed that the prepared CQDs and heterozygous CQDs were homogeneous, with controllable luminescence, and the electrochemiluminescence signal was stable. In addition, the polyhedral structure of nangolden particles (AuNPs) was successfully prepared by the reducibility of CQDs, which was not with the traditional method of AuNPs. .2. a CQDs based electrochemiluminescence sandwich immunosensor for the measurement of carcinoembryonic antigen (CEA), an electrochemiluminescence sandwich immunosensor based on CQDs for the measurement of CEA is successfully prepared. The polymer (PDA-AgNPs) of polydopamine and silver nanoparticles (PDA-AgNPs) is used as a platform to immobilizing an antibody (Ab1), and it can also improve the electron conduction rate.CQD. S is immobilized on the polyethyleneimine (PEI) functionalized graphene oxide (GO) through the amino group, then AuNPs is immobilized on CQDs-PEI-GO and then bonded to the two anti (Ab2). By combining CEA with Ab1 and Ab2, CQDs can be fixed on the surface of the electrode to produce electrochemiluminescence signals. Under optimal experimental conditions, the ECL intensity and CEA concentration of the sensor are in the best experimental condition. The linear equation is linear, the linear equation is IECL=3380.3+1138.4 LG cCEA/ng mL-1, the correlation coefficient is R=0.9989, the minimum detection limit of CEA is 1.67 PG mL-1 (S/N=3). The sensor is also successfully applied to the detection of CEA in the actual sample. The sensor has good sensitivity, stability, specificity and reproducibility, and is expected to be applied to.3 in the diagnosis of disease. An electrochemiluminescence sensor based on the co reaction of CQDs and Ru (bpy) 32+ for the detection of bisphenol A (BPA) was used to prepare a ECL sensor based on CQDs and Ru (bpy) 32+ co reaction assay BPA. -GO can not only load a large number of CQDs but also accelerate the electronic transmission between the electrode and the solution, and then improve the sensitivity of the detection. Then, the modified electrode is used in the solution containing Ru (bpy) 32+ to detect the BPA. on the ECL of the ECL of the Ru (bpy) 32+/CQDs luminescence system by BPA. The sensor is used to detect BPA. The linear range of 5-1000 nmol mL-1, the detection limit of 2 nmol mL-1. experiments proved that the sensor has good stability, high sensitivity and lower detection limit and wider linear range.4. based on carbon quantum dots (CQDs) as a co reactants of the Ru (Ru (bpy) 32+) electrochemical luminescence (Ru (bpy) 32+) for the high sensitivity detection of carcinoembryonic antigen (CEA) A sandwich immune ECL sensor based on the co reaction of CQDs and Ru (bpy) 32+ was prepared. CQDs was immobilized on PEI-GO, and the CQDs-PEI-GO complex was used to fix an anti Ab1. mesoporous silicon (MSN) load Ru. On N. Here, CQDs is a co reactant of Ru (bpy) 32+. Under the best experimental conditions, the linear range of the sensor is 1 pg. ML-1-1000ng. ML-1, and the detection limit is 0.33 PG mL-1 (S/N=3). The sensor has good specificity, stability and reproducibility.
【學(xué)位授予單位】：聊城大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2016
【分類號】：O657.3

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