本文選題：動(dòng)態(tài)表面增強(qiáng)拉曼光譜 + 最佳熱點(diǎn)��； 參考：《中國(guó)科學(xué)技術(shù)大學(xué)》2017年碩士論文

【摘要】：表面增強(qiáng)拉曼光譜(SERS)自20世紀(jì)70年代發(fā)現(xiàn)以來,由于能夠提供分子的指紋信息、非破壞性、以及超靈敏性特點(diǎn),SERS技術(shù)已經(jīng)成為一個(gè)強(qiáng)有力的分析工具,可應(yīng)用于化學(xué)、生物以及環(huán)境分析。近些年來,本課題組發(fā)展的動(dòng)態(tài)表面增強(qiáng)拉曼光譜(D-SERS)憑借其高靈敏性,重現(xiàn)性和穩(wěn)定性以及實(shí)時(shí)檢測(cè)的特點(diǎn)也逐漸受到關(guān)注。眾所周知,納米材料的形貌對(duì)SERS增強(qiáng)效果有很大的影響,各項(xiàng)異性的納米粒子(納米星、三角形、管狀等)作為增強(qiáng)基底靈敏性很高,但重現(xiàn)性很低。在SERS檢測(cè)中,獲得重現(xiàn)性好、可靠性高的檢測(cè)結(jié)果,合成單分散的納米粒子是至關(guān)重要的。本論文主要是基于單分散的納米粒子作為SERS基底,結(jié)合D-SERS方法的諸多優(yōu)點(diǎn)來開展的一系列工作。第一章簡(jiǎn)單的介紹了 SERS的基本概念、原理和基底材料,SERS在醫(yī)學(xué)、單分子檢測(cè)、公共安全方面的應(yīng)用。重點(diǎn)介紹了 D-SERS的發(fā)現(xiàn)、發(fā)展過程以及D-SERS的特征和優(yōu)點(diǎn),目前存在的問題和研究思路。第二章是基于D-SERS能夠?qū)崿F(xiàn)實(shí)時(shí)檢測(cè)的特點(diǎn),再結(jié)合雙組份分析法來實(shí)時(shí)研究?jī)煞N同分異構(gòu)體2,2'-Bpy和4,4'-Bpy的競(jìng)爭(zhēng)吸附。通過D-SERS的實(shí)時(shí)監(jiān)測(cè)研究發(fā)現(xiàn)2,2'-Bpy和4,4'-Bpy的吸附是一個(gè)動(dòng)態(tài)競(jìng)爭(zhēng)的過程。此動(dòng)態(tài)吸附的變化過程在普通的干態(tài)方法下是無法檢測(cè)到的,D-SERS實(shí)時(shí)檢測(cè)的特點(diǎn)為研究分子的競(jìng)爭(zhēng)吸附提供了方法。第三章提出了 "最佳熱點(diǎn)"的概念,并基于最佳熱點(diǎn)建立了可靠的定量分析方法。采用原位小角X射線散射技術(shù)(SAXS)實(shí)時(shí)地追蹤"最佳熱點(diǎn)"的形成過程,結(jié)果表明在單分散納米溶膠蒸發(fā)的過程中確實(shí)形成了 "最佳熱點(diǎn)"。采用4-巰基吡啶(4-mpy)作為內(nèi)標(biāo)分子,結(jié)晶紫(CV)作為模型分子進(jìn)行方法驗(yàn)證,將D-SERS最佳熱點(diǎn)處的最強(qiáng)信號(hào)強(qiáng)度用于統(tǒng)計(jì)分析。結(jié)果表明,CV的相對(duì)強(qiáng)度與濃度的負(fù)對(duì)數(shù)成線性關(guān)系,即可以實(shí)現(xiàn)定量檢測(cè)。最終,通過這種方法,兩種毒品搖頭丸(MDMA)、a-甲基色胺二鹽酸鹽(a-MT)以及三聚氰胺都可以實(shí)現(xiàn)定量檢測(cè)。第四章是在第三章的基礎(chǔ)上進(jìn)一步進(jìn)行的探索。運(yùn)用D-SERS過程中的"最佳熱點(diǎn)"結(jié)合免內(nèi)標(biāo)(internal standards-free)的方法實(shí)現(xiàn)對(duì)一類特殊分子的定量檢測(cè)。這類特殊的分子是指具有較大散射截面和對(duì)稱性結(jié)構(gòu)的分子,例如三苯甲烷染料。CV是廉價(jià)的三苯甲烷染料,它能幫助魚類有效對(duì)抗真菌和寄生蟲感染。但由于這些染料對(duì)人類有致突變和致畸作用,在水產(chǎn)養(yǎng)殖中是禁止使用的。因此,準(zhǔn)確測(cè)定三苯甲烷染料的濃度是至關(guān)重要的。結(jié)果表明,采用這種方法可以實(shí)現(xiàn)對(duì)三苯甲烷染料的定量檢測(cè)。第五章主要是在第三和第四章內(nèi)容的基礎(chǔ)上來探索"最佳熱點(diǎn)"的可控性。最佳熱點(diǎn)處具有很多的優(yōu)點(diǎn),然而最佳熱點(diǎn)的存在時(shí)間非常短,變化非常快,而且這一過程是不可逆的。因此,我們希望采用不同的方法將最佳熱點(diǎn)的存在時(shí)間延長(zhǎng),并通過小角X射線散射(SAXS)實(shí)時(shí)追蹤方法的可行性。結(jié)果表明通過封閉和液封都可以實(shí)現(xiàn)對(duì)熱點(diǎn)的控制,這對(duì)D-SERS乃至SERS而言都有著極其重要的意義。
[Abstract]:Since the surface enhanced Raman spectroscopy (SERS) was discovered in 1970s, because of its ability to provide molecular fingerprint information, nondestructive, and super sensitive characteristics, SERS technology has become a powerful analytical tool that can be applied to chemical, biological and environmental analysis. In recent years, the dynamic surface enhanced Raman light (SERS) developed by our group has been developed. D-SERS, with its high sensitivity, reproducibility and stability as well as the characteristics of real-time detection, has been paid more attention. It is known that the morphology of nanomaterials has a great influence on the enhancement of SERS. The sensitivity of various nanoparticles (nanoscale, triangle, tube, etc.) is very high, but the reproducibility is very low. The detection of SERS is very low. In order to obtain good reproducibility and high reliability detection results, the synthesis of monodisperse nanoparticles is very important. This paper is based on a series of work based on the advantages of the single dispersed nanoparticles as the SERS substrate and the D-SERS method. The first chapter briefly introduces the basic concepts, principles and substrate materials, SER of the SERS. The application of S in medicine, single molecule detection and public safety. This paper focuses on the discovery of D-SERS, the development process, the characteristics and advantages of D-SERS, the existing problems and research ideas. The second chapter is based on the characteristics of the real-time detection based on the D-SERS, and then combines the dual component analysis method to study the two isomers in real time, 2,2'-Bpy and the real time. The competitive adsorption of 4,4'-Bpy. Through real-time monitoring of D-SERS, it is found that the adsorption of 2,2'-Bpy and 4,4'-Bpy is a dynamic competition process. The dynamic adsorption process can not be detected under the ordinary dry state method. The characteristic of real-time detection of D-SERS provides a method for studying the competitive adsorption of molecules. The third chapter puts forward the "most" The concept of "good hot spot" and a reliable quantitative analysis method based on the best hot spot were established. In situ small angle X ray scattering (SAXS) was used to track the formation process of "the best hot spot" in real time. The results showed that the best hot spot was formed in the process of evaporation of monodisperse nanossols. 4- mercapto pyridine (4-Mpy) was used as the internal standard. Crystal violet (CV) is used as a model molecule to verify the strongest signal intensity at the best hot spot of D-SERS. The results show that the relative intensity of CV is linear with the negative logarithm of the concentration, that is, the quantitative detection can be achieved. Finally, two kinds of drug ecstasy (MDMA) and a- methyl chromamine two hydrochloride (a-MT) are obtained by this method. And melamine can be quantified. The fourth chapter is a further exploration on the basis of the third chapter. Using the "best hot spot" in the D-SERS process and the method of internal standards-free, the quantitative detection of a class of special molecules is realized. This special molecule refers to the large scattering cross section and symmetry. Structural molecules, such as the triphenyl methane dye.CV, are cheap triphenyl methane dyes that help fish effectively against fungal and parasitic infections. But because these dyes have mutagenic and teratogenic effects on human beings, it is forbidden to use in aquaculture. Therefore, it is essential to determine the concentration of three benzyl dyes accurately. The fifth chapter is mainly based on the content of the third and fourth chapters to explore the controllability of "the best hot spot". The best hot spot has many advantages, however, the best hot spot has a very short time, very fast change, and this process is irreversible. Therefore, we hope to use different methods to extend the time of the best hot spot, and through the feasibility of the small angle X ray scattering (SAXS) real-time tracking method. The result shows that both the sealing and the liquid seal can realize the control of the hot spot, which is of great significance for the D-SERS and even the SERS.
【學(xué)位授予單位】：中國(guó)科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O657.37

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