本文選題：碳量子點(diǎn)　切入點(diǎn)：石墨烯量子點(diǎn)　出處：《安徽師范大學(xué)》2015年博士論文　論文類型：學(xué)位論文

【摘要】：熒光碳量子點(diǎn)(CQDs,2004年首次報(bào)道),這種零維碳納米材料因其獨(dú)特的性能一直是人們持續(xù)關(guān)注的熱點(diǎn)。與傳統(tǒng)的半導(dǎo)體量子點(diǎn)和熒光染料相比,水溶性好、易于功能化、耐光漂白、毒性低、生物相容性好,這些諸多優(yōu)勢使其在生物學(xué)和生物醫(yī)學(xué)研究中越來越顯示出極大的應(yīng)用潛力。然而,目前制得的碳量子點(diǎn)在長波發(fā)射和量子產(chǎn)率方面存在明顯不足。根據(jù)現(xiàn)有的文獻(xiàn)報(bào)道,碳量子點(diǎn)的“發(fā)射最大波長”(即發(fā)射強(qiáng)度或效率最大所對(duì)應(yīng)的發(fā)射波長)大都小于500nm,且熒光量子產(chǎn)率較低,大多數(shù)裸碳量子點(diǎn)都小于10%。因此,研究發(fā)展不需要復(fù)雜的鈍化及后處理過程的簡單方法,可控制備普適于生物成像應(yīng)用的具有高熒光量子產(chǎn)率的近紅區(qū)發(fā)射碳量子點(diǎn)是十分必要的。本工作主要集中在碳量子點(diǎn)制備的方法學(xué)研究及其生物分析應(yīng)用兩方面。首先,通過改進(jìn)碳源氧化方式及實(shí)驗(yàn)條件控制,摸索了一種快速深度氧化不同碳源方法,在2-3小時(shí)反應(yīng)時(shí)間快速獲得了“發(fā)射最大波長”在538 nm、熒光量子產(chǎn)率為50%和“發(fā)射最大波長”在600 nm、熒光量子產(chǎn)率為18%的石墨烯量子點(diǎn);并系統(tǒng)研究了石墨烯量子點(diǎn)高熒光量子產(chǎn)率的紅光發(fā)射行為與其組成、粒徑、表面態(tài)的內(nèi)在聯(lián)系與規(guī)律,旨在加深對(duì)碳量子點(diǎn)發(fā)光機(jī)制的理解。然后,基于綠光發(fā)射的石墨烯量子點(diǎn)的pH敏感光學(xué)性質(zhì),構(gòu)建了尿素的熒光傳感檢測系統(tǒng),并應(yīng)用于血液中尿素的檢測;同時(shí),將紅光發(fā)射石墨烯量子點(diǎn)應(yīng)用于細(xì)胞成像,考察了其抗生物基質(zhì)熒光干擾的性能;并將紅光發(fā)射石墨烯量子點(diǎn)包埋于葉酸靶向脂質(zhì)體中,成功實(shí)現(xiàn)了細(xì)胞表面葉酸受體過度表達(dá)的MCF-7細(xì)胞的靶向成像,為石墨烯量子點(diǎn)的靶向標(biāo)記及傳感提供一種簡單可行的方法。論文共分為三章,具體內(nèi)容如下:第一章,首先對(duì)碳量子點(diǎn)的性質(zhì)、制備方法及應(yīng)用進(jìn)行綜述,并在分析了熒光碳量子點(diǎn)的國內(nèi)外研究背景及發(fā)展趨勢基礎(chǔ)上,確定了論文設(shè)想。第二章,采用高濃度硝酸,對(duì)常用硝酸氧化方法作了大的改進(jìn)。以酒精燈灰為碳源,合成了高量子產(chǎn)率(50%)的綠光石墨烯量子點(diǎn),對(duì)其形貌、組成進(jìn)行相關(guān)表征,探討其高量子產(chǎn)率的熒光機(jī)制。第三章,通過改換活性炭為碳源,合成高量子產(chǎn)率紅光發(fā)射的石墨烯量子點(diǎn),通過對(duì)其形貌、組成等相關(guān)表征,探討了其高量子產(chǎn)率和長波發(fā)射的發(fā)光機(jī)制。第四章,研究了綠光發(fā)射石墨烯量子點(diǎn)的熒光性質(zhì),依據(jù)其靈敏的pH依賴熒光性質(zhì),構(gòu)建了簡單、靈敏的尿素?zé)晒鉁y定體系,并應(yīng)用于人體血液中尿素的測定。第五章,將合成得到高量子產(chǎn)率紅光發(fā)射石墨烯量子點(diǎn)應(yīng)用于細(xì)胞成像,考察了其抗生物基底背景熒光干擾和生物相容性能第六章,基于葉酸-葉酸受體介導(dǎo)的靶向性,脂質(zhì)體優(yōu)越的生物相容性。制備了熒光石墨烯量子點(diǎn)葉酸靶向脂質(zhì)體,通過熒光光譜和投射電鏡對(duì)其進(jìn)行了表征。初步實(shí)現(xiàn)了其靶向熒光成像。最后對(duì)本論文工作進(jìn)行總結(jié)并提出下一步研究工作思路。
[Abstract]:Fluorescent carbon quantum dots (CQDs, first reported in 2004), the zero dimensional carbon nano materials because of its unique properties has been a hot spot of continuing concern. With the traditional semiconductor quantum dots and fluorescent dye, good water solubility, easy functionalization, light bleaching, low toxicity, good biocompatibility, these many advantages make it in biological and biomedical research increasingly shows great potential. However, the current carbon quantum dots prepared in the presence of long wavelength and quantum yield is obviously insufficient. According to the existing literature reports, the emission maximum wavelength of CQDS "(i.e. the emission wavelength emission intensity or maximum efficiency the corresponding) are mostly less than 500nm, and the fluorescence quantum yield is low, most of the bare carbon dots are smaller than 10%.. Therefore, the research does not require the development of simple method for complex passivation and postprocessing process, controllable preparation for students Application of NIR imaging material with high quantum yield of fluorescence emission of carbon quantum dots is very necessary. This work is focused on the methods of carbon quantum dots prepared by research and applications in biological analysis in two aspects. First, through the improvement of carbon oxidation method and experimental condition control, to find a fast oxidation different carbon source method, in 2-3 hours of fast response time obtained "emission maximum wavelength" at 538 nm, the fluorescence quantum yield of 50% and the maximum emission wavelength at 600 nm, the fluorescence quantum yield of gqds 18%; red emission behavior and studied graphene quantum dots with high fluorescence quantum yield its composition, particle size, inherent relation and regularity of surface states, to deepen the understanding of the mechanism of carbon quantum dots. Then, pH sensitive optical properties of graphene quantum dot emission based on the construction of the urea Fluorescence sensing detection system, detection and application in blood urea; at the same time, the red emission of gqds application in cell imaging, the performance of its anti biological matrix fluorescence interference was investigated; and the red emission of graphene quantum dots embedded in folate targeted liposomes, successfully targeting cell imaging the surface of the folate receptor expression of MCF-7 cells, providing a simple and feasible method for graphene quantum dots targeting and sensing. The thesis is divided into three chapters, the specific contents are as follows: the first chapter firstly, properties of carbon quantum dots, preparation method and application are reviewed, and based on the analysis of the the background and development trend of domestic and international research on the fluorescent carbon quantum dots, the conceive of the thesis. The second chapter, the high concentration of nitrate, nitric acid oxidation method to commonly used made big improvements. The alcohol lamp ash as carbon source, high quantum yield of synthesis The rate of (50%) green graphene quantum dots, the morphology, composition were characterized, and investigate the mechanism of high fluorescence quantum yield. In the third chapter, through the change of activated carbon as carbon source, graphene quantum dots synthesized high quantum yield red emission, based on the morphology, composition and other related characterization, discussed the high quantum yield and long wave emission luminescence mechanism. The fourth chapter studies the green emission fluorescence properties of graphene quantum dots, on the basis of the sensitive pH dependent fluorescence properties, constructed a simple, sensitive fluorescent urea determination system, and applied to the determination of urea in the blood of people. In the fifth chapter, the synthesis of high the red emission quantum yield of graphene quantum dots used in cell imaging, investigated the compatibility of the sixth chapter of the anti biological substrate background fluorescence and biology to based on folic acid - receptor mediated liposome target, superior biological compatibility A fluorescent graphene quantum dot folate targeted liposome was prepared. It was characterized by fluorescence and projection electron microscopy. The targeted fluorescence imaging was initially achieved. Finally, the work of this paper was summarized and the next research ideas were proposed.

【學(xué)位授予單位】：安徽師范大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2015
【分類號(hào)】：O657.3;O613.71

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