本文關(guān)鍵詞： 表面增強(qiáng)拉曼散射 樣品前處理 食品快檢 農(nóng)殘 地溝油　出處：《吉林大學(xué)》2017年博士論文　論文類型：學(xué)位論文

【摘要】：傳統(tǒng)實(shí)驗(yàn)室分析技術(shù),如色譜、質(zhì)譜技術(shù)可針對(duì)復(fù)雜體系進(jìn)行多組分定性、定量分析,但分析周期較長(zhǎng)、分析結(jié)果滯后,不能及時(shí)有效監(jiān)控食品和環(huán)境的安全現(xiàn)狀。所以,快速、高效、準(zhǔn)確的食品分析技術(shù)是現(xiàn)階段食品快速檢測(cè)領(lǐng)域面臨的十分棘手的問題。表面增強(qiáng)拉曼散射(SERS)是一種基于散射原理的指紋圖譜技術(shù),與其他測(cè)試技術(shù)相比,具有樣品用量少、測(cè)試速度快、分辨率高、靈敏度高等特點(diǎn),可用于溶劑體系下痕量物質(zhì)的超靈敏檢測(cè),尤其在現(xiàn)場(chǎng)定性檢測(cè)方面越來越受到人們的關(guān)注,發(fā)展一種簡(jiǎn)單有效的前處理方法與SERS檢測(cè)技術(shù)結(jié)合是食品快檢領(lǐng)域的當(dāng)務(wù)之急。本課題基于表面增強(qiáng)拉曼散射技術(shù),利用磁性材料發(fā)展高選擇性、環(huán)境友好的樣品前處理方法與小型化拉曼光譜儀有效結(jié)合,為發(fā)展快速有效的食品檢測(cè)與監(jiān)測(cè)提供新的技術(shù)手段,進(jìn)而為食品安全保駕護(hù)航。研究?jī)?nèi)容主要包括以下三個(gè)方面:1、采用層層組裝的方法制備了一種多功能磁性石墨烯基SERS基底:Fe_3O_4@GO@Ag。該基底同時(shí)具有固相萃取和SERS檢測(cè)的功能,利用該基底發(fā)展了一種新型的預(yù)處理、檢測(cè)方法稱為:表面磁膜固相萃取-表面增強(qiáng)拉曼散射技術(shù)(Surface Magnetic Solid Phase Extraction-SERS:SMSPE-SERS),SMSPE-SERS技術(shù)集目標(biāo)分子的表面萃取、分離與檢測(cè)于一體。利用該基底對(duì)果皮、蔬菜表面農(nóng)藥殘留的萃取、分離到檢測(cè)整個(gè)過程僅需15 min,對(duì)福美雙和噻菌靈兩種農(nóng)殘的最低檢出限分別達(dá)到:0.48 ng/cm2和4 ng/cm2。2、Fe_3O_4@GO@Ag三元復(fù)合材料可集萃取、分離、檢測(cè)于一體,但是分步法制備該三元SERS基底,制備工藝復(fù)雜,制備時(shí)間較長(zhǎng),重復(fù)制備對(duì)工藝參數(shù)要求較高,不適合工藝放大,因此我們嘗試使用一鍋法的工藝制備三元SERS基底。以乙酰丙酮鐵作為鐵源,乙二醇為溶劑,NaAc為還原劑,聚乙烯亞胺為靜電組裝劑。分別探討了NaAc和AgNO_3用量對(duì)Fe_3O_4和AgNPs在石墨烯表面的負(fù)載量,按照優(yōu)化的實(shí)驗(yàn)配比進(jìn)行了工藝放大研究。對(duì)一鍋法制備的三元SERS基底進(jìn)行了SERS活性研究,結(jié)果顯示,一鍋法制備的三元基底與多步自組裝法具有同樣的SERS活性。3、地溝油的甄別是分析化學(xué)和食品安全領(lǐng)域的重要難題,辣椒堿是目前鑒定地溝油的重要外源性標(biāo)記物,辣椒堿的檢測(cè)技術(shù)目前主要由HPLC-MS實(shí)現(xiàn),本論文基于表面增強(qiáng)共振拉曼散射(SERRS)技術(shù),利用分子的衍生化,建立了地溝油中的外源性標(biāo)記物:辣椒堿的超靈敏檢測(cè)方法。通過使用特殊的衍生化試劑,從SERRS機(jī)理出發(fā),使目標(biāo)分子的最大吸收波長(zhǎng)與激發(fā)光波長(zhǎng)最大程度重疊,再利用具有磁聚集功能的磁性納米粒子作為SERS基底,可實(shí)現(xiàn)辣椒堿的超靈敏檢測(cè),檢測(cè)限可達(dá)到1.0×10-9 M,該方法為地溝油的鑒定提供了一種簡(jiǎn)單、快速、超靈敏的分析方法。
[Abstract]:Traditional laboratory analysis techniques, such as chromatography and mass spectrometry, can be used for qualitative and quantitative analysis of complex systems, but the analysis period is longer and the analysis results lag behind. Not timely and effective monitoring of food and environmental safety status. So, fast, efficient. Accurate food analysis technology is a very difficult problem in the field of rapid food detection. Surface enhanced Raman scattering (SERS) is a fingerprint technology based on scattering principle. Compared with other testing techniques, it has the advantages of less sample consumption, faster testing speed, higher resolution and higher sensitivity. It can be used for the hypersensitive detection of trace substances in solvent system. Especially in the field of qualitative testing, people pay more and more attention to it. It is an urgent task to develop a simple and effective pre-processing method combined with SERS detection technology. Based on surface-enhanced Raman scattering technology, magnetic materials are used to develop high selectivity. The combination of environmentally friendly sample pretreatment method and miniaturized Raman spectrometer provides a new technique for the development of rapid and effective food detection and monitoring. And then for food safety escort. The research mainly includes the following three aspects: 1. A kind of multifunctional magnetic graphene base SERS substrate: Fe3O\ +\\%\%\\%\\\. A new kind of pretreatment was developed by using the substrate. The detection method is called surface magnetic film solid phase extraction-surface enhanced Raman scattering (. Surface Magnetic Solid Phase Extraction-SERS: SMSPE-SERS. The SMSPE-SERS technique integrates the surface extraction, separation and detection of the target molecules. The substrate is used to extract pesticide residues on the pericarp and vegetable surfaces. The detection time was only 15 minutes, and the minimum detection limits for Fumex and thiabendazole were 0. 48 ng/cm2 and 4 ng/cm2.2, respectively. Fe_3O_4@GO@Ag ternary composites can be extracted, separated and detected in one body, but the preparation process of the ternary SERS substrate is complicated and the preparation time is longer. The repeated preparation requires higher technological parameters and is not suitable for the process amplification. Therefore we try to prepare ternary SERS substrate by one-pot process with iron acetylacetone as Tie Yuan and ethylene glycol as solvent. NaAc was used as reducing agent and polyethylene imine as electrostatic assembler. The loading amount of NaAc and AgNO_3 on the surface of graphene was studied respectively. The SERS activity of ternary SERS substrate prepared by one-pot method was studied according to the optimized experimental ratio. The ternary substrate prepared by one-pot method has the same SERS activity as multi-step self-assembly method. The screening of gutter oil is an important problem in the field of analytical chemistry and food safety. Capsaicin is an important external marker for the identification of gutter oil. The detection technology of capsaicin is mainly realized by HPLC-MS at present. In this paper, surface enhanced resonance Raman scattering (SERRS) technique is used to detect capsaicin. A new method for the detection of capsaicin in gutter oil was established by molecular derivation. By using special derivatization reagent, the mechanism of SERRS was studied. The maximum absorption wavelength of the target molecule overlaps with the excitation wavelength to the greatest extent, and then the magnetic nanoparticles with magnetic aggregation function are used as the SERS substrate to realize the hypersensitive detection of capsaicin. The detection limit can reach 1.0 脳 10 ~ (-9) M. this method provides a simple, rapid and hypersensitive method for the identification of gutter oil.
【學(xué)位授予單位】：吉林大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2017
【分類號(hào)】：TS207.3;O657.37

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