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硅基SERS基底优化及对临床耳聋突变致病基因和实体水中汞离子的检测

发布时间:2018-07-20 21:46
【摘要】:硅纳米材料具备很多优异的特性,在分析化学和生物学等学科领域中受到广泛的关注。本论文基于电化学反应原理通过调节和优化反应溶液硝酸银的pH值,在单晶硅片表面原位还原生长银纳米粒子,制备得到粒径分布均匀的硅基材料(Silver Nanoparticles-decorated Silicon wafer,AgNPs@Si),并对不同pH值条件下得到的AgNPs@Si基底进行表面增强拉曼散射(Surface-Enhanced Raman Scattering,SERS)效应的科学研究。以优化后的AgNPs@Si材料作为高效的SERS基底,我们进一步发展了一种新型的硅基SERS检测策略,实现对基因突变性耳聋致病基因和湖水中汞离子含量的分析检测。本论文的主要研究内容有:1、用氢氟酸蚀刻法制备AgNPs@Si SERS基底。系统研究了反应溶液硝酸银的pH值对AgNPs@Si表面形貌(粒子尺寸和分布情况)及其SERS强度的影响。随着硝酸银溶液的pH值从1增加到12,银纳米粒子尺寸不断增大(40-120 nm),趋向于均匀分布,材料具有较高的SERS信号强度;当硝酸银溶液的pH值继续增加到13和14时,银纳米粒子出现尺寸不均一现象,部分粒子聚集严重。相应的,AgNPs@Si材料的拉曼强度逐渐减弱。在硝酸银溶液的pH值为12时制备得到的AgNPs@Si材料具有最强的SERS信号强度,重现性良好。2、选择最优条件下的AgNPs@Si材料(p H值为12)作基底,发展了茎环结构DNA辅助的硅基SERS检测平台并对DNA及实际体系中的耳聋突变致病基因进行灵敏性和特异性分析检测。其最低检测浓度低至500 fM,具有良好的灵敏性、特异性和重现性。3、继续选取最佳条件下制备得到的AgNPs@Si材料(pH值为12)作为基底,我们构建了一种高效的SERS生物传感器,完成了对毒性汞离子的分析检测。在八种干扰离子存在的条件下对汞离子的检测极限最低可达到100 fM,同时可实现对实体湖水中汞离子的高特异性和灵敏性检测。AgNPs@Si材料具有制备成本低、操作过程简单和重现性良好等特点,我们希望这种硅基SERS平台能在环境和生物分析等实际检测领域得到广泛应用。
[Abstract]:Silicon nanomaterials have attracted much attention in analytical chemistry and biology due to their excellent properties. Based on the electrochemical reaction principle, silver nanoparticles were prepared by in situ reduction of silver nanoparticles on the surface of single crystal silicon wafer by adjusting and optimizing the pH value of silver nitrate solution. Silver Nanoparticles-decorated Silicon wafer wafers (AgNPs) have been prepared and the surface-enhanced Raman scattering (SERS) effects have been studied on the AgNPs @ Si substrates at different pH values. Using the optimized AgNPs @ Si as a highly efficient SERS substrate, we further developed a novel Si-based SERS detection strategy for the detection of mutagenic deafness genes and mercury ion content in lake water. The main research contents of this thesis are as follows: (1) the substrate of AgNPs Si is prepared by hydrofluoric acid etching. The effects of the pH value of silver nitrate in the reactive solution on the surface morphology (particle size and distribution) and SERS strength of AgNPs @ Si were systematically studied. With the increase of pH value of silver nitrate solution from 1 to 12, the size of silver nanoparticles increases (40-120 nm), tends to uniform distribution, and the material has higher signal intensity of SERS), when the pH value of silver nitrate solution continues to increase to 13 and 14:00, The size of silver nanoparticles is uneven, and some of the particles gather seriously. The Raman intensity of the corresponding AgNPs @ Si material decreases gradually. When the pH value of silver nitrate solution is 12:00, the AgNPs @ Si material has the strongest SERS signal intensity and good reproducibility. The optimum condition is that the AgNPs Si material (pH = 12) is selected as the substrate. A silicon-based SERS platform was developed for DNA assisted detection of stem ring structure and the sensitivity and specificity of DNA and deafness mutation genes in the actual system were analyzed. Its lowest detection concentration is as low as 500fM, and it has good sensitivity, specificity and reproducibility. We have constructed an efficient SERS biosensor by selecting the AgNPs @ Si material (pH = 12) prepared under the optimum conditions as the substrate. The analysis and detection of toxic mercury ions were completed. In the presence of eight kinds of interference ions, the detection limit of mercury ions can be as low as 100 fm, and the high specificity and sensitivity of mercury ions in solid lake water can be detected. Since the operation process is simple and reproducible, we hope that the Si-based SERS platform can be widely used in the field of environmental and biological analysis.
【学位授予单位】:苏州大学
【学位级别】:硕士
【学位授予年份】:2015
【分类号】:R764.43;O657.37

【共引文献】

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