中文题名: | 金纳米材料比色法在毛细管电泳检测树枝状大分子及可视分子逻辑门体系构建中的应用 |
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保密级别: | 公开 |
论文语种: | 中文 |
学科代码: | 070302 |
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学生类型: | 硕士 |
学位: | 理学硕士 |
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学位年度: | 2018 |
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提交日期: | 2018-06-28 |
答辩日期: | 2018-05-29 |
外文题名: | Application of Gold Nanomaterial-Based Colorimetry in Capillary Electrophoretic Determination of PAMAM dendrimers and in Construction of Molecular Logic Gates |
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中文摘要: |
毛细管电泳是一类以高压电场为驱动力,以毛细管为分离通道,基于待分析物淌度差异的一种高效分离分析技术。其具有高效、快速、低样品消耗、自动化等优点,是继气相色谱和高效液相色谱之后分析科学领域的又一重要角色。依据待分析物性质选择适合的检测手段,并将其与毛细管电泳相偶联,是实现高效分离检测的重要基础。
金纳米颗粒具有极高的摩尔消光系数,基于其建立的纳米金比色法灵敏度高,便捷性强,无需大型仪器,是一种极具应用潜力的分析检测方法。然而其目标专一性在很大程度上依赖于复杂的表面修饰,在实际应用中所表现出的选择性往往不甚理想。
本文的研究工作围绕基于金纳米材料的比色法展开,共分为两部分。其一,将具有高分离效能的毛细管电泳与高灵敏度的纳米金比色法相结合,建立了一种新型的分离检测方法。其二,以金纳米棒刻蚀比色反应为基础,建立了一多功能分子逻辑门体系。
本论文共分为三个章节。第一章为前言,主要对毛细管电泳、纳米金比色法的基本原理、树枝状大分子的检测和应用以及基于纳米金的逻辑门进行了综合概述。
第二章为毛细管电泳-纳米金比色法联用装置用于检测人尿中的PAMAM树枝状大分子。搭设了一新型双鞘流接口,通过将分离缓冲液与纳米金反应液相互隔离开来,实现了毛细管电泳分离装置与纳米金柱后比色检测单元的有机结合。以加标于人尿样本的PAMAM G1.0,G2.0,G3.0树枝状大分子为模式分析物对该联用装置进行了可行性验证。利用正交实验法对毛细管电泳分离缓冲液进行了最优化选取;通过控制变量法,逐一优化了柱后纳米金反应液的pH、离子强度、浓度以及流速。在最优条件下,PAMAM G1.0,G2.0和G3.0在8 min内实现基线分离,检出限分别为0.5, 1.2和2.6 μg?mL-1。该方法的灵敏度甚至优于高效液相色谱-荧光法和质谱法。实验结果显示,该系统对于复杂基质中具有相似性质的目标分析物的快速、灵敏检测具有极佳的适应性和广阔的应用前景。
第三章为基于碘刻蚀金纳米棒构建的比色分子逻辑门体系。通过将巯基化合物、金汞齐对金纳米棒的保护效果以及铜离子(Ⅱ)对刻蚀的促进作用结合起来,建立了五个分子逻辑门,分别为AND, NOR, XNOR, YES和IMPLY。该逻辑门体系在执行运算时伴随金纳米棒溶胶由红至蓝的颜色变化,可实现裸眼观测或光谱测量。此外,该体系中的双输入IMPLY逻辑门可实现对Hg2+和Cu2+两种重金属离子的同时灵敏检测,光谱学检出限均符合EPA标准。
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外文摘要: |
This thesis consists of three chapters. The first chapter mainly provides a comprehensive overview of fundamentals of capillary electrophoresis, gold nanoparticle-based colorimetry, the application and determination of PAMAM dedrimers and the application of gold nanomaterials in logic gate construction.
In the second chapter, we report a method integrating capillary electrophoresis (CE) and gold nanoparticle aggregation-based colorimetry (AuNP@A). By using a dual-sheath interface, the running buffer was isolated from the colorimetric reaction solution so that CE and AuNP@A would not interfere with each other. The proof-of-concept was validated by assay of polyamidoamine (PAMAM) dendrimers that were fortified in human urine samples. The factors influencing the CE-AuNP@A performances were investigated and optimized. Under the optimal conditions, the dendrimers were separated within 8 minutes, with detection limits of 0.5, 1.2 and 2.6 μg?mL-1 for PAMAMs G1.0, G2.0 and G3.0, respectively. The sensitivity of CE-AuNP@A was comparable to or even better than those of liquid chromatography-fluorimetry and liquid chromatography-mass spectrometry. The results suggested that the proposed strategy can be applied to facile and quick determination of analytes of similar properties in complex matrices.
In the third chapter, a multi-logic gate platform was designed based on iodine-mediated etching of gold nanorods (AuNRs). By utilizing the anti-etching effects of sulphydryl compounds and Au-Hg amalgams as well as the etching-promoting effect of Cu2+, we built five logic gates namely, AND, NOR, XNOR, YES and IMPLY. Operations of these logic gates were accompanied by red-to-blue color changes of the AuNR colloids, enabling naked-eye observation or spectroscopic measurements. In addition, we demonstrated the simultaneous, sensitive detection of Hg2+ and Cu2+ with the binary IMPLY gate.
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参考文献总数: | 0 |
馆藏号: | 硕070302/18005 |
开放日期: | 2019-07-09 |