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基于量子點(diǎn)的雙發(fā)射二氧化硅納米微球的制備及其分析應(yīng)用研究

發(fā)布時間:2018-05-31 11:20

  本文選題:離子印跡 + 鎘離子 ; 參考:《浙江工業(yè)大學(xué)》2016年碩士論文


【摘要】:半導(dǎo)體量子點(diǎn),又稱半導(dǎo)體納米晶,因其具有優(yōu)秀的光學(xué)性質(zhì),在分析檢測方面受到越來越多的關(guān)注。相比于有機(jī)染料,量子點(diǎn)具有亮度高、耐光性強(qiáng)、發(fā)射光譜窄、尺寸可調(diào)等優(yōu)點(diǎn)。近年來,量子點(diǎn)作為熒光探針被廣泛應(yīng)用于金屬離子、有機(jī)小分子、氣體、蛋白質(zhì)和DNA等的檢測。相比于單發(fā)射波長的熒光量子點(diǎn),比率熒光探針因其具有更高的靈敏度,能夠進(jìn)行自我矯正以及可視化檢測受到了更大的關(guān)注。為了提高量子點(diǎn)熒光比率探針在金屬離子檢測方面的選擇性以及在生物樣品方面的可視化檢測能力,本論文設(shè)計合成了兩種雙發(fā)射納米粒子作為熒光比率探針。主要工作如下:(1)結(jié)合“turn-on”模型和“離子印跡”技術(shù),我們設(shè)計合成了雙發(fā)射的量子點(diǎn)雜化納米粒子,并將它用于水中Cd~(2+)的熒光比率檢測。我們通過將綠色熒光的CdSe量子點(diǎn)共價偶聯(lián)到包埋紅光CdTe量子點(diǎn)的硅球表面,合成了比率探針。接著,我們利用EDTA對CdSe量子點(diǎn)表面進(jìn)行化學(xué)刻蝕,CdSe的綠色熒光隨之猝滅,同時在CdSe表面產(chǎn)生Cd~(2+)的特異性識別位點(diǎn)。當(dāng)加入Cd~(2+)后,Cd~(2+)對CdSe表面進(jìn)行修復(fù),綠色熒光逐漸恢復(fù),而紅色熒光保持不變,隨著Cd~(2+)離子濃度的增加,我們就可以明顯觀察到探針溶液發(fā)生了從紅色到綠色的顏色變化。在最優(yōu)實(shí)驗(yàn)條件下,該比率探針檢測Cd~(2+)的檢測限達(dá)25 nM(S/N=3),線性范圍為0.1到9μM。因此,該比率熒光探針提供了一種靈敏度和選擇性很高的Cd~(2+)離子檢測方法。(2)構(gòu)建強(qiáng)大的熒光強(qiáng)度比例和顏色可調(diào)的雙/多發(fā)射熒光納米粒子作為高選擇性的熒光比率探針具有重要意義。我們通過將綠色量子點(diǎn)原位生長到包埋紅色量子點(diǎn)二氧化硅納米顆粒的表面,將兩種不同尺寸的CdTe量子點(diǎn)在空間上分開,組裝合成了一種新型的二氧化硅包覆的雙發(fā)射雜化納米粒子CdTe@SiO_2@CdTe@SiO_2。只要簡單地控制反應(yīng)時的回流時間或者改變量子點(diǎn)的前驅(qū)體的濃度,我們就可以控制改變該納米粒子的熒光強(qiáng)度的比值和熒光顏色。相比于之前報道的CdTe@SiO_2@CdTe納米顆粒,我們合成的CdTe@SiO_2@CdTe@SiO_2納米粒子表現(xiàn)出更強(qiáng)的光穩(wěn)定性、化學(xué)穩(wěn)定性以及生物相容性。最后,我們證明了該雙發(fā)射熒光二氧化硅雜化粒子可以通過熒光能量轉(zhuǎn)移機(jī)制,來精確地檢測金納米顆粒濃度。
[Abstract]:Semiconductor quantum dots (QDs), also known as semiconductor nanocrystals, have attracted more and more attention in analysis and detection because of their excellent optical properties. Compared with organic dyes, quantum dots have the advantages of high brightness, strong light resistance, narrow emission spectrum and adjustable size. In recent years, quantum dots (QDs) have been widely used as fluorescent probes for the detection of metal ions, organic small molecules, gases, proteins and DNA. Compared with single emission wavelength fluorescence quantum dots, ratio fluorescence probes have attracted more attention because of their high sensitivity, self-correction and visual detection. In order to improve the selectivity of quantum dot fluorescence ratio probe in metal ion detection and visual detection ability in biological samples, two kinds of double emission nanoparticles were designed and synthesized as fluorescence ratio probes in this paper. The main work is as follows: (1) combined with "turn-on" model and "ion imprinting" technique, we have designed and synthesized double emission quantum dot hybrid nanoparticles, and used it to measure the fluorescence ratio of Cd~(2 in water. A ratio probe was synthesized by covalently coupling green fluorescent CdSe quantum dots to the surface of silicon spheres embedded with red CdTe quantum dots. Then we use EDTA to chemically etch the green fluorescence of CdSe on the surface of CdSe quantum dots and produce the specific recognition sites of Cd~(2 on the surface of CdSe. After the addition of Cd~(2), the surface of CdSe was repaired, and the green fluorescence was gradually restored, but the red fluorescence remained unchanged. With the increase of the concentration of Cd~(2), we observed that the probe solution changed from red to green. Under the optimal experimental conditions, the detection limit of the ratio probe for Cd~(2 is up to 25 nm / s / N ~ (3 +) and the linear range is from 0.1 渭 m to 9 渭 M. Therefore, This ratio fluorescence probe provides a highly sensitive and selective Cd~(2) ion detection method. 2) to construct a strong fluorescence intensity ratio and color adjustable double / multiple emission fluorescent nanoparticles as a high selective fluorescence ratio. The probe is of great significance. By in situ growing green quantum dots onto the surface of silica nanoparticles embedded in red quantum dots, we separate two CdTe quantum dots of different sizes from each other in space. A new type of silica coated double emission hybrid nano-particle CdTeSiO2 was assembled and synthesized. By simply controlling the reflux time during the reaction or changing the concentration of the precursor of the quantum dot, we can control the ratio of fluorescence intensity and the fluorescence color of the nanoparticles. Compared with the previously reported CdTe@SiO_2@CdTe nanoparticles, the synthesized CdTe@SiO_2@CdTe@SiO_2 nanoparticles exhibit stronger photostability, chemical stability and biocompatibility. Finally, we prove that the dual-emission fluorescent silica hybrid particles can accurately detect the concentration of gold nanoparticles by fluorescence energy transfer mechanism.
【學(xué)位授予單位】:浙江工業(yè)大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2016
【分類號】:O657.3;O613.72

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本文編號:1959443


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