【摘要】：硅納米材料具備很多優(yōu)異的特性,在分析化學(xué)和生物學(xué)等學(xué)科領(lǐng)域中受到廣泛的關(guān)注。本論文基于電化學(xué)反應(yīng)原理通過調(diào)節(jié)和優(yōu)化反應(yīng)溶液硝酸銀的pH值,在單晶硅片表面原位還原生長銀納米粒子,制備得到粒徑分布均勻的硅基材料(Silver Nanoparticles-decorated Silicon wafer,AgNPs@Si),并對不同pH值條件下得到的AgNPs@Si基底進(jìn)行表面增強(qiáng)拉曼散射(Surface-Enhanced Raman Scattering,SERS)效應(yīng)的科學(xué)研究。以優(yōu)化后的AgNPs@Si材料作為高效的SERS基底,我們進(jìn)一步發(fā)展了一種新型的硅基SERS檢測策略,實(shí)現(xiàn)對基因突變性耳聾致病基因和湖水中汞離子含量的分析檢測。本論文的主要研究內(nèi)容有:1、用氫氟酸蝕刻法制備AgNPs@Si SERS基底。系統(tǒng)研究了反應(yīng)溶液硝酸銀的pH值對AgNPs@Si表面形貌(粒子尺寸和分布情況)及其SERS強(qiáng)度的影響。隨著硝酸銀溶液的pH值從1增加到12,銀納米粒子尺寸不斷增大(40-120 nm),趨向于均勻分布,材料具有較高的SERS信號強(qiáng)度;當(dāng)硝酸銀溶液的pH值繼續(xù)增加到13和14時(shí),銀納米粒子出現(xiàn)尺寸不均一現(xiàn)象,部分粒子聚集嚴(yán)重。相應(yīng)的,AgNPs@Si材料的拉曼強(qiáng)度逐漸減弱。在硝酸銀溶液的pH值為12時(shí)制備得到的AgNPs@Si材料具有最強(qiáng)的SERS信號強(qiáng)度,重現(xiàn)性良好。2、選擇最優(yōu)條件下的AgNPs@Si材料(p H值為12)作基底,發(fā)展了莖環(huán)結(jié)構(gòu)DNA輔助的硅基SERS檢測平臺并對DNA及實(shí)際體系中的耳聾突變致病基因進(jìn)行靈敏性和特異性分析檢測。其最低檢測濃度低至500 fM,具有良好的靈敏性、特異性和重現(xiàn)性。3、繼續(xù)選取最佳條件下制備得到的AgNPs@Si材料(pH值為12)作為基底,我們構(gòu)建了一種高效的SERS生物傳感器,完成了對毒性汞離子的分析檢測。在八種干擾離子存在的條件下對汞離子的檢測極限最低可達(dá)到100 fM,同時(shí)可實(shí)現(xiàn)對實(shí)體湖水中汞離子的高特異性和靈敏性檢測。AgNPs@Si材料具有制備成本低、操作過程簡單和重現(xiàn)性良好等特點(diǎn),我們希望這種硅基SERS平臺能在環(huán)境和生物分析等實(shí)際檢測領(lǐng)域得到廣泛應(yīng)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.
【學(xué)位授予單位】：蘇州大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：R764.43;O657.37

【共引文獻(xiàn)】

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本文編號：2134888