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荧光性的金属纳米簇合成及传感性能研究

发布时间:2018-11-18 18:10
【摘要】:近些年来,荧光标记技术已经深入到人类研究的各个方面,如生物医药领域等。荧光标记材料分为有机染料、半导体量子点、复合荧光纳米粒子以及贵金属纳米簇,由于后三种荧光材料的粒子尺寸都在纳米级别上,我们又将其合称为荧光纳米标记材料。因其具有优良的光化学性质,赢得了广大研究者的关注,并成为新一代的荧光标记材料。我们所说的金属纳米簇,是指由Au、Ag或Cu等金属的几个至几十个原子组成的一类新型的荧光纳米材料。它们的粒子尺寸一般小于2nm,因其优异的光谱和光物理性质而受到科学家们的青睐。其中,迄今为止,利用脱氧核糖核酸(DNA)为基本骨架,合成的贵金属纳米簇已广泛应用于荧光成像、生物化学传感、纳米器件、抗菌剂、环境监测等诸多领域。本论文则利用不同的DNA模板合成Ag NCs,实现对DNA序列的选择性识别,并利用荧光银纳米簇为探针检测Hg2+,同时对荧光铜纳米粒子进行了初步的研究。本文的主要研究内容和实验结论如下:1.采用(CNG)n序列DNA为模板,以NaBH4为还原剂合成具有荧光性质的银纳米簇,这是一种快速、高效、传统的合成银纳米簇的方法。通过紫外可见光谱和荧光光谱等表征方法研究了此类银纳米簇(Ag NCs)的荧光性质,并通过有机分子拥挤条件进一步提高了以DNA为模板合成的荧光性银纳米簇的选择性和灵敏度,为检测(CGG)序列提供了一种新的可能性。实验结果表明:(CNG)n序列为模板合成的银纳米簇的荧光发射对DNA序列选择依赖性的顺序为GCT≈A,这种选择性顺序在不同长度(CNG)n序列上依然适用。此外,此方法优越性在于利用有机分子提高了Ag NCs选择性识别(CGG)的灵敏度,进一步说明了该实验方法的高效、便捷以及合理性。2. 主要以Three-way DNA为模板,以NaBH4为还原剂合成荧光银纳米簇,优化了反应物摩尔比、反应时间等合成条件。通过荧光光谱等手段研究了该类型银纳米簇的荧光性质,并简单介绍了DNA/Ag NCs在检测汞离子中的应用。实验结果表明:含有胞嘧啶碱基的Three-way DNA能更有效地合成Ag NCs,这进一步说明银纳米簇的合成强烈依赖于DNA序列,而且合成的纳米簇还可以用来检测Hg2+离子。3. 以一些均聚物即含多个相同碱基组成的单链DNA为模板,选用抗坏血酸钠作还原剂来合成荧光性的铜纳米粒子,利用荧光稳态的方法研究了DNA碱基对铜纳米粒子生长的选择性以及稳定性的影响。实验结果表明:含有多个胸腺嘧啶碱基的ss-DNA模板能够有效的合成荧光性质的铜纳米粒子,且其荧光强度随着碱基长度的增加而增加。
[Abstract]:In recent years, fluorescent labeling techniques have been applied to all aspects of human research, such as biomedicine. Fluorescent labeling materials are divided into organic dyes semiconductor quantum dots composite fluorescent nanoparticles and noble metal nanoclusters. Because the size of the latter three fluorescent materials are at the nanometer level we call them fluorescent nanolabelling materials. Because of its excellent photochemical properties, it has attracted the attention of researchers and become a new generation of fluorescent labeling materials. The metal nanoclusters are a new kind of fluorescent nanomaterials composed of several to dozens of atoms of metals such as Au,Ag or Cu. They are generally smaller than 2 nm in size and are favored by scientists for their excellent spectral and photophysical properties. Up to now, the synthetic noble metal nanoclusters have been widely used in many fields, such as fluorescence imaging, biochemical sensing, nano-devices, antimicrobial agents, environmental monitoring and so on, using deoxyribonucleic acid (DNA) as the basic skeleton. In this thesis, Ag NCs, was synthesized by different DNA templates to realize the selective recognition of DNA sequences, and the fluorescent silver nanoclusters were used as probes to detect Hg2, and the fluorescent copper nanoparticles were studied preliminarily. The main research contents and experimental results are as follows: 1. Silver nanoclusters with fluorescence properties were synthesized by using (CNG) n sequence DNA as template and NaBH4 as reducing agent. This is a fast, efficient and traditional method for the synthesis of silver nanoclusters. The fluorescence properties of silver nanoclusters (Ag NCs) were studied by UV-Vis and fluorescence spectra. The selectivity and sensitivity of fluorescent silver nanoclusters synthesized using DNA as template were further improved under the condition of organic molecular crowding, which provided a new possibility for the detection of (CGG) sequences. The experimental results show that the order of fluorescence emission dependence on DNA sequence of silver nanoclusters synthesized by: (CNG) n sequence is GCT 鈮,

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