本文選題：鍺摻雜的碳點 + 氮摻雜的碳點��； 參考：《西南大學(xué)》2016年碩士論文

【摘要】：碳點(carbon dots)一般是指粒徑小于10 nm的碳納米材料。由于其獨特的光學(xué)性質(zhì)和優(yōu)良的生物相容性,碳點已經(jīng)成為超越熒光分子和量子點的材料,引起了無數(shù)研究者的關(guān)注,并且已被用于生物成像、分析檢測、光電催化,以及能量轉(zhuǎn)移等方面。然而,對于碳點的發(fā)光機(jī)理、不同光學(xué)性質(zhì)碳點的合成、以及在碳點表面引入不同的功能化基團(tuán)的相關(guān)報道還較少。為了更好地了解碳點并開發(fā)其實用價值,我們應(yīng)該對這些方面進(jìn)行更深入的研究與探討。本文合成了一系列用檸檬酸(CA)作為碳源的碳點。在表征其發(fā)光性質(zhì)、探索其發(fā)光機(jī)制的基礎(chǔ)上,做了以下研究:(1)將鍺摻雜的碳點作為一種新型熒光探針用于可視化動態(tài)監(jiān)視汞離子入侵細(xì)胞。本文首次將檸檬酸與羧乙基鍺倍半氧化物分別做為碳源與鍺源,用一種簡單快速(15 min)的碳化法合成了鍺元素?fù)诫s的碳點(GeCDs)。不同于大多數(shù)碳點的發(fā)射波長對激發(fā)波長的依賴,GeCDs的發(fā)射波長不依賴激發(fā)波長。GeCDs具有細(xì)胞毒性低、生物相溶性好、化學(xué)性質(zhì)穩(wěn)定的特點。更重要的是,GeCDs能夠在金銀花露溶液或細(xì)胞溶液等極其復(fù)雜的環(huán)境中與汞離子特異結(jié)合。此外,GeCDs還可作為一種新型探針,用于在人喉癌細(xì)胞(HEp-2)中實時監(jiān)測汞離子入侵細(xì)胞的過程,以及可視化監(jiān)測汞離子引起的細(xì)胞重大生理變化。(2)通過調(diào)節(jié)表面狀態(tài)可控合成具有不同光學(xué)性質(zhì)的氮摻雜的碳點本文以檸檬酸與鹽酸胍為原料合成了一系列碳材料,其中一部分表現(xiàn)出發(fā)射波長依賴激發(fā)波長的性質(zhì)(EDE),另一部分表現(xiàn)出發(fā)射波長不依賴激發(fā)波長的光學(xué)性質(zhì)(EIE)。同時,這些碳材料具有化學(xué)性質(zhì)穩(wěn)定、對細(xì)胞的毒性低、生物相容性好的特點。通過對碳點表面狀態(tài)的調(diào)節(jié),可以改變碳點的光學(xué)性質(zhì)(例如EDE,EIE,熒光量子產(chǎn)率等)。對實驗數(shù)據(jù)的分析表明,碳點表現(xiàn)出不同光學(xué)性質(zhì)的原因在于表面狀態(tài)的差異。如果碳點表面被鹽酸胍完全鈍化,碳點表現(xiàn)為EIE特征,量子產(chǎn)率可以高達(dá)60.5%。如果表面鈍化程度低,碳點表現(xiàn)為EDE特征。分析還發(fā)現(xiàn),汞離子可以與這些碳點特異性地結(jié)合,致使碳點熒光猝滅。該現(xiàn)象可以用電子轉(zhuǎn)移能級重疊解釋,即碳點LUMO能級上的電子轉(zhuǎn)移到汞離子上,而不是回到HOMO能級,致使碳點不能發(fā)射出熒光。由于本文合成的碳點化學(xué)性質(zhì)穩(wěn)定,且與汞離子有特殊作用,故可作為一種有效的熒光探針,可視化監(jiān)測細(xì)胞內(nèi)的汞離子濃度。
[Abstract]:Carbon point (carbon dots) usually refers to carbon nanomaterials with diameter less than 10 nm. Because of their unique optical properties and excellent biocompatibility, carbon dots have become materials beyond fluorescent molecules and quantum dots, which have attracted the attention of numerous researchers and have been used in biological imaging, analytical detection, photocatalysis, And energy transfer and so on. However, there are few reports on the luminescence mechanism of carbon points, the synthesis of carbon spots with different optical properties and the introduction of different functionalized groups on the surface of carbon spots. In order to better understand the carbon point and develop its practical value, we should study these aspects more deeply. A series of carbon spots with citric acid (CA) as carbon source have been synthesized. On the basis of characterizing its luminescence properties and exploring its luminescence mechanism, the following studies have been done: (1) the germanium doped carbon point is used as a new fluorescent probe to visualize the dynamic monitoring of mercury ion invasion cells. It is the first time that citric acid and carboxyethyl germanium semicoxide are used as carbon source and germanium source respectively. GE doped carbon spots (GeCDs) were synthesized by a simple and fast carbonization method (15 min). Different from the emission wavelengths of most carbon spots, the emission wavelengths of GeCDs do not depend on the excitation wavelengths. GeCDs have the characteristics of low cytotoxicity, good biocompatibility and stable chemical properties. More importantly, GeCDs can specifically bind to mercury ions in extremely complex environments such as honeysuckle solution or cell solution. In addition, GeCDs can be used as a new probe for real-time monitoring of mercury ion invasion in human laryngeal cancer cells (HEp-2). Visual monitoring of cellular physiological changes induced by mercury ions. (2) nitrogen doped carbon spots with different optical properties were synthesized by adjusting the surface state. A series of carbon materials were synthesized from citric acid and guanidine hydrochloride. Some of them show the properties of emission wavelength dependent on excitation wavelength (EDE) and the other part show optical property of emission wavelength independent of excitation wavelength (EIE). At the same time, these carbon materials have the characteristics of stable chemical properties, low cytotoxicity and good biocompatibility. By adjusting the surface state of the carbon point, the optical properties of the carbon point can be changed (such as EDEE, fluorescence quantum yield, etc.). The analysis of the experimental data shows that the difference of surface states is the reason for the different optical properties of carbon spots. If the surface of the carbon spot is completely passivated by guanidine hydrochloride, the carbon spot is characterized by EIE, and the quantum yield can reach 60.5%. If the surface passivation is low, the carbon point is characterized by EDE. It is also found that mercury ions can specifically bind to these carbon spots, resulting in fluorescence quenching of carbon spots. This phenomenon can be explained by the overlap of electron transfer energy levels, that is, the electrons on the LUMO level of the carbon point transfer to the mercury ion instead of returning to the Homo level, resulting in the emission of fluorescence from the carbon point. Due to the stable chemical properties of the carbon points synthesized in this paper and its special role with mercury ions, it can be used as an effective fluorescence probe to visually monitor the concentration of mercury ions in cells.
【學(xué)位授予單位】：西南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2016
【分類號】：O613.71;O657.3

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