發(fā)布時間：2018-02-08 11:09

  本文關(guān)鍵詞： 硼氮共摻雜碳點 氮硫共摻雜碳點 汞離子 姜黃素 還原型谷胱甘肽　出處：《山西醫(yī)科大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：目的:熒光碳點(CDs)作為一種新型的碳納米材料因具有優(yōu)良的光學(xué)性能、優(yōu)越的生物相容性、良好的水溶性、較低的細胞毒性等優(yōu)點被廣泛用于熒光探針、光催化劑、生物成像和熒光化學(xué)傳感器等領(lǐng)域。雖然碳點的優(yōu)點很多,但是傳統(tǒng)的碳點熒光量子產(chǎn)率相對較低,極大限制了其在化學(xué)傳感、藥物載體、生物成像等領(lǐng)域的發(fā)展。研究者們利用各種方法來提高碳點的量子產(chǎn)率,發(fā)現(xiàn)將N、S、P等雜原子與碳點摻雜可以有效提高碳點的量子產(chǎn)率。因此,制備高量子產(chǎn)率的摻雜碳點并開發(fā)其在分析測試中的應(yīng)用具有現(xiàn)實意義。方法:本文利用微波加熱法成功制備了硼氮共摻雜碳點(BNCDs)和氮硫共摻雜碳點(NSCDs)。通過透射電鏡(TEM)、X射線衍射法(XRD)、傅里葉變換紅外光譜(FT-IR)、X射線光電子能譜(XPS)等技術(shù)對這兩種摻雜碳點的形狀、粒徑大小、官能團及元素組成等進行了表征。利用紫外-可見吸收光譜(UV-Vis)和熒光光譜考察了摻雜碳點的光學(xué)性質(zhì)。BNCDs的熒光強度隨著溶液中Hg~(2+)或姜黃素濃度的增加顯著降低,利用此現(xiàn)象分別建立了檢測Hg~(2+)和姜黃素的方法�；贖g~(2+)對NSCDs熒光猝滅及還原型谷胱甘肽(GSH)使NSCDs-Hg~(2+)體系熒光恢復(fù)的特性,建立了檢測GSH的“開關(guān)”型(turnoff/on)熒光探針。結(jié)果:分別對BNCDs和NSCDs的形態(tài)、元素組成及官能團進行了表征。以BNCDs為熒光探針,對Hg~(2+)和姜黃素進行了定量測定。Hg~(2+)的檢出限(LOD)是2.3nM,線性范圍是0.04～22.00 μM。此外,姜黃素的檢出限和線性范圍分別為65 nM、0.2～12.5 μM。該方法被成功用于自來水和湖水樣品中Hg~(2+)的測定,加標回收率在99.8～101.8%之間。對尿樣和血樣中姜黃素的含量進行了測定,回收率是96.5～105.5%。我們還構(gòu)建了一種基于NSCDs的“開關(guān)”型熒光探針,實現(xiàn)了 GSH的微量測定。向NSCDs溶液中引入Hg~(2+)后,NSCDs熒光明顯被猝滅,此時NSCDs-Hg~(2+)體系處于熒光“關(guān)閉”的狀態(tài)。向NSCDs-Hg~(2+)體系加入GSH溶液后,NSCDs熒光得到恢復(fù),此時體系處于熒光“打開”的狀態(tài),這一過程可用于GSH的測定,檢出限為52 nM,線性范圍是0.5～34.0μM。結(jié)論:基于Hg~(2+)和姜黃素對BNCDs熒光的猝滅,分別建立了實際水樣中Hg~(2+)和實際樣品中姜黃素的檢測方法。初步推斷Hg~(2+)對BNCDs的熒光猝滅主要為靜態(tài)猝滅過程,姜黃素對BNCDs熒光猝滅主要是內(nèi)濾光效應(yīng)和動態(tài)猝滅。利用Hg~(2+)使NSCDs熒光猝滅和GSH對NSCDs-Hg~(2+)體系熒光恢復(fù)的過程,構(gòu)建了“開關(guān)”型熒光探針,用于實際尿樣和血樣中GSH的檢測,獲得滿意的結(jié)果。探討了 NSCDs熒光猝滅和恢復(fù)的機理。Hg~(2+)與NSCDs相互作用的過程主要為動態(tài)猝滅。由于GSH對Hg~(2+)的親和力很強,向NSCDs-Hg~(2+)體系加入GSH后,GSH與Hg~(2+)形成穩(wěn)定的配合物,從而使NSCDs熒光得到恢復(fù)。
[Abstract]:Objective: as a new carbon nanomaterial, fluorescent carbon dots (CDS) have been widely used as fluorescent probes and photocatalysts for their excellent optical properties, excellent biocompatibility, good water solubility and low cytotoxicity. Although the advantages of carbon dots are many, the fluorescence quantum yields of traditional carbon dots are relatively low, which greatly limits their applications in chemical sensing, drug carriers, and so on. The researchers used various methods to improve the quantum yield of carbon dots, and found that doping hetero atoms such as Nu Schip with carbon dots can effectively improve the quantum yield of carbon dots. It is of practical significance to prepare doped carbon dots with high quantum yield and to develop their applications in analysis and measurement. Methods: in this paper, boron nitrogen co-doped carbon dots (BNCDs) and nitrogen-sulfur co-doped carbon dots (NSCDss) were successfully prepared by microwave heating. The shape of the two doped carbon spots was studied by means of electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The size of particle size, functional group and elemental composition were characterized. The optical properties of the doped carbon sites were investigated by UV-Visand fluorescence spectra. The fluorescence intensity of the doped carbon dots decreased with the increase of Hg~(2) or curcumin concentration in the solution. Using this phenomenon, a method for the detection of Hg~(2) and curcumin was developed. The fluorescence quenching of NSCDs and the fluorescence recovery of NSCDs-Hg~(2 by reduced glutathione (Glutathione) were based on Hg~(2. A "switch" fluorescence probe for the detection of GSH was established. Results: the morphology, elemental composition and functional groups of BNCDs and NSCDs were characterized, respectively. BNCDs was used as fluorescence probe. The detection limit of Hg~(2) and curcumin was 2.3nM and the linear range of curcumin was 0.04 ~ 22.00 渭 M. in addition, the detection limit and linear range of curcumin were 65 nm ~ 0.2n ~ (12.5 渭 m), respectively. The method has been successfully applied to the determination of Hg~(2 in tap water and lake water samples. The recoveries of curcumin in urine and blood samples were determined in the range of 99.8 ~ 101.8%. The recoveries of curcumin in urine and blood samples were 96. 5 ~ 105.5%. We also constructed a "switch" fluorescent probe based on NSCDs. The microdetermination of GSH was realized. The fluorescence of GSH was obviously quenched after the introduction of Hg~(2 into NSCDs solution, and the fluorescence of NSCDs-Hg~(2) system was in the state of "off". The fluorescence of NSCDs was recovered after adding GSH solution to the NSCDs-Hg~(2 system. This process can be used for the determination of GSH with a detection limit of 52 nm and a linear range of 0.5 渭 m ~ 34.0 渭 M. conclusion: based on Hg~(2) and curcumin, the fluorescence of BNCDs can be quenched. Methods for the determination of curcumin in real water samples and curcumin samples were established respectively. The fluorescence quenching of BNCDs by Hg~(2) was mainly a static quenching process. The fluorescence quenching of BNCDs by curcumin was mainly internal filter effect and dynamic quenching. By using Hg~(2 to quench the fluorescence of NSCDs and GSH to restore the fluorescence of NSCDs-Hg~(2) system, a "switch" fluorescence probe was constructed for the detection of GSH in real urine and blood samples. The mechanism of fluorescence quenching and recovery of NSCDs was studied. The process of interaction between GSH and NSCDs was mainly dynamic quenching. Because of the strong affinity of GSH to Hg~(2), the NSCDs-Hg~(2) system was added to GSH to form a stable complex. Thus, the fluorescence of NSCDs was restored.
【學(xué)位授予單位】：山西醫(yī)科大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O657.3;TB383.1

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