【作者】 张秀秀；

【导师】 吴志勇；

【作者基本信息】 东北大学 ， 分析化学， 2019， 硕士

【摘要】 纸基分析装置(PAD)作为一种新型的分析检测平台,自2007年首次报道以来已经广泛应用于环境监测,食品控制,医疗诊断和药物控制等多个领域。通常情况下,以纸张作为低成本诊断平台具有简单便携,快速制造,易于操作,成本低,无毒性等优点。这在工业化程度较低,专业人员和实验室分析技术匮乏的发展中国家和偏远地区来说是非常重要的。然而,PAD的灵敏度较低限制了其应用性能。因此,开发灵敏度较高的纸基分析装置以实现目标分析物的即时检测是非常重要的。本文的第一章主要介绍了纸基分析装置的基本发展历程,常见的检测方法以及在环境监测,食品控制及医疗诊断方面的应用。另外,着重阐述了纸基分析装置中比色法和化学发光分析法的研究现状。第二章将Griess反应与纸基电动堆积(ES)方法相结合,利用智能手机在简单的PAD上实现了无色亚硝酸根的比色分析。首先,本实验尝试对侧通道的位置,堆积时间和比色时间等实验条件进行优化。在最优实验条件下,该实验尝试探究了该方法的分析灵敏度和富集效果,检出限为0.073 μg/mL,使亚硝酸根的检出能力与文献报道相比提高了 10倍,使得信号强度提高了约160倍。为验证该方法的可行性,本实验将上述方法应用于人体唾液样品、饮用水和环境水样中亚硝酸根含量的检测,加标回收率为91.0%～108.7%。该方法与其他仪器分析方法(分光光度法等)相比,具有传统纸基分析方法的各种优点。另外,又在一定程度上提高了传统PAD方法的分析灵敏度。这在一定程度上为无色目标分析物的高灵敏现场测定提供了新的思路。第三章成功地将灵敏度较高的化学发光检测法与场放大电动堆积相结合,利用一种价廉、微型集成化的高灵敏光电检测模块构建了一个便携式化学发光PAD检测系统。首先,本实验探究了电压,背景电解质浓度,鲁米诺浓度,过氧化氢浓度及发光试剂中氢氧化钠的浓度对发光信号的影响。在如上最优条件下,本实验利用氯化血红素探究了该方法的检测灵敏度和选择性能,使得信号强度提高了约13倍,检出限为0.58 nmol/L。在此基础上成功实现了药物和人血清中氯化血红素的检测,加标回收率为84.0%～106.0%。该方法在保持PAD系统的便携和现场检测等特点的同时,在一定程度上进一步提高了纸基分析装置的检测灵敏度。更多还原

【Abstract】 As a new on-site analytical platform,paper-based analytical device(PAD)has been widely used in environmental monitoring,food quality control and clinical diagnostic and drug control since it was introduced by Whitesides in 2007.The major advantages of PAD include simplicity,portability,easy to operate,low cost and so on.This is important for developing countries and remote areas where industrialization degree is low and requires professional and laboratory analytical techniques for portable and real-time detection.However,compared with laboratory based analytical instruments,the sensitivity of PAD is often limited for low abundant analytes,which hinders their extensive applications.Improving the sensitivity of PAD is necessary to achieve on-site detection of target analytes.In the first chapter of this work,we mainly introduced the development of PAD,major detection methods and the application in environmental monitoring,food quality control and clinical diagnostic.In addition,the research status of colorimetric and chemiluminescence in PAD was emphasized.In the second chapter,we attempted to combine the Griess reaction with electrokinetic stacking(ES)to achieve the colorimetric analysis of the colorless nitrite on simple PAD using a smartphone.Firstly,the experimental conditions such as the position of the side channel,the electrokinetic stacking time and the colorimetric time were optimized,respectively.Under the optimal conditions,we tried to explore the analytical sensitivity and enrichment effect of the method,which the limit of detection(LOD)was 0.073 μg/mL.The sensitivity of nitrite was 160-fold increased.The limit of detection was 10 times lower than the reported,and closed to that achieved by a desktop spectrophotometer.In order to verify the feasibility of the method,we applied the method to the detection of nitrite in human saliva samples,drinking water and environmental water samples with recovery in the range of 91.0%～108.7%.This method has various advantages of the conventional paper-based analysis method compared with other instrumental analysis methods(spectrophotometry and so on).In addition,the sensitivity of traditional paper-based analysis methods has been improved.This method provides a method for highly sensitive on-site determination of colorless target analytes.In the third chapter,a sensitive PAD system with chemiluminscence(CL)detection and electrokinetic preconcentration was introduced,and the performance was demonstrated by the detection of hemin.A commercial available low cost and miniaturized optical detection module was used for the CL detection.Firstly,we investigated the effects of the applied voltage,the concentration of background electrolyte solution,luminol,hydrogen peroxide and sodium hydroxide in the luminescent reagent on the chemiluminescence signal.Under the optimal conditions,the detection sensitivity and selectivity of the method using hemin was explored,and the sensitivity was 13-fold increased.The limit of detection(LOD)was 0.58 nmol/L.On this basis,we successfully achieved the detection of hemin in common iron supplements and human serum with recovery in the range of 84.0%～116.0%.The sensitivity of the paper-based analysis device was improved with this method while characteristics of the portable and on-site detection of the PAD system was maintained.更多还原