基于SERS技术检测三种管制药物的研究

发布时间：2018-06-20 22:08

本文选题：表面增强拉曼光谱 + SERS基底　；参考：《哈尔滨工业大学》2017年硕士论文

【摘要】：近些年来,药物滥用引起的社会安全问题频发,对患者的人身安全造成极大地危害。如何有效的检测和监控药物、预防药物的非法流通、滥用,已成为我国面临的一个重要问题。目前,大部分针对药物滥用的检测方法往往具有成本高、效率低、预处理过程复杂、对检测环境有一定要求、检测的设备体积大,不便携等缺点。表面增强拉曼散射(SERS)技术自上世纪九十年代以来,已广泛应用于食品安全、药品鉴定及材料分析等各个领域,作为新兴的分析检测技术,SERS凭借极高的灵敏度及不受水的干扰等优点,在对药物滥用的现场、快速、实时检测中表现出极大地实际应用价值。在本研究中,我们对SERS增强基底进行了制备及表征,并对三种管制药物SERS试验的检测条件进行了实验探讨,以确定每种滥用药物的最理想实验条件,最后通过实验完成对氢溴酸东莨菪碱、盐酸异丙嗪、硫酸阿托品三种药物的SERS检测和半定量分析工作。对滥用药物的监察及现场快速的检测具有很重要地意义。首先我们使用高斯(Gaussian)软件中含有的密度泛函理论(DFT)计算方法,对氢溴酸东莨菪碱、盐酸异丙嗪、硫酸阿托品三种药物进行计算,确定其在B3LYP杂化函数中的不同的基组和校正因子,并优化分子结构,经计算后获取三种药物的理论拉曼光谱。将理论结果与实验检测得到的药物固体拉曼光谱及SERS光谱三者进行比较,再结合Gaussview软件对每种药物的拉曼光谱特征峰及其对应的振动模式进行归属工作,为后续实验根据拉曼特征峰确定相应分子做铺垫。然后利用化学还原法,制备了形貌均一的银溶胶SERS活性基底,并利用场发射扫描电子显微镜(SEM)和动态光散射仪对其性能进行表征,结果显示银溶胶中纳米颗粒尺寸分布均匀,基底自身无拉曼信号,不会对实验结果产生干扰的。基于银溶胶SERS活性基底,对它的批次间稳定性进行研究,以确保SERS检测的可重复性。此外,对承载平台的衬底材料进行研究,确定一种简单高效的疏水反光衬底,用于进行SERS实验。最后基于银溶胶SERS增强基底,建立一种对氢溴酸东莨菪碱、盐酸异丙嗪、硫酸阿托品水溶液的无需预处理、所需检测时间短的SERS检测方法。通过实验研究不同促凝剂(无机盐)对拉曼信号强度增强的影响,确定每种药物使用的最理想促凝剂,并对三种药品进行SERS检测。研究了不同浓度梯度的三种药品水溶液的SERS光谱,分别得到检测极限可至0.1μg/m L、0.61μg/m L、0.5μg/m L。此外,对三种药物SERS方法的可重复性进行了研究,经计算回收率分别可达到98.5%~109.7%、96.5%~108.8%、98.3%~107.4%。这个方法自身具有操作简便、检测时间短、检测结果准确的优势,结果显示SERS技术在滥用药物监查、检测方面具有极大地应用前景。
[Abstract]:In recent years, social security problems caused by drug abuse have caused great harm to patients' personal safety. How to effectively detect and monitor drugs and prevent the illegal circulation and abuse of drugs has become an important problem in China. At present, most of the detection methods for drug abuse often have the disadvantages of high cost, low efficiency, complex pretreatment process, certain requirements to the detection environment, large volume of detection equipment, not portable and so on. Surface enhanced Raman scattering (SERS) technology has been widely used in food safety, drug identification and material analysis since the 1990s. As a new analytical and detection technology, SERS has shown great practical value in the field of drug abuse, rapid and real-time detection, because of its high sensitivity and no interference from water. In this study, the SERS enhanced substrate was prepared and characterized, and the detection conditions of three kinds of controlled drugs for SERS test were discussed in order to determine the optimal experimental conditions for each drug abuse. Finally, SERS detection and semi-quantitative analysis of scopolamine hydrobromide, promethazine hydrochloride and atropine sulfate were carried out. It is of great significance to monitor drug abuse and to detect drug abuse quickly on the spot. First of all, we use the density functional theory (DFT) method contained in Gao Si Gaussian-based software to calculate three kinds of drugs: scopolamine hydrobromide, promethazine hydrochloride and atropine sulfate. The different basis groups and correction factors in the B3LYP hybrid function were determined and the molecular structure was optimized. The theoretical Raman spectra of the three drugs were obtained after calculation. The theoretical results were compared with the experimental results, and the Raman spectra and SERS spectra were compared. The characteristic peaks of Raman spectra and their corresponding vibrational modes of each drug were assigned by Gaussview software. For the subsequent experiments according to the Raman characteristic peak to determine the corresponding molecules as a cushion. Then the SERS active substrates with uniform morphology were prepared by chemical reduction method. The properties of SERS active substrates were characterized by field emission scanning electron microscopy (SEM) and dynamic light scattering (DLS). The results showed that the size distribution of silver sol nanoparticles was uniform. The substrate itself has no Raman signal and will not interfere with the experimental results. Based on the active substrate of silver sol SERS, the stability between batches was studied to ensure the repeatability of SERS detection. In addition, a simple and efficient hydrophobic reflective substrate is determined for SERS experiments. Finally, based on the silver sol SERS enhanced substrate, a new SERS detection method for scopolamine hydrobromide, promethazine hydrochloride and atropine sulfate solution was established. The effects of different coagulants (inorganic salts) on the enhancement of Raman signal intensity were studied experimentally. The optimal coagulant for each drug was determined and three drugs were detected by SERS. The SERS spectra of three kinds of drug aqueous solutions with different concentration gradients were studied. The detection limit was up to 0.1 渭 g / m L ~ (-1) 0.61 渭 g / m ~ (-1) or 0.5 渭 g / m ~ (-1) 路m ~ (-1). In addition, the repeatability of three SERS methods was studied. The recoveries of the three drugs were 98.5 and 109.70.96. 5and 108.8and 107.4respectively. This method has the advantages of simple operation, short detection time and accurate detection results. The results show that SERS technology has great application prospect in drug abuse monitoring.
【学位授予单位】：哈尔滨工业大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：R969;O657.37

【相似文献】