论文总字数：26409字

摘 要

一氧化碳（CO）被认为是第二种气体递质与生理和病理过程存在着密切关系。从外界摄入过量的CO，会导致中毒，而内部存在的CO是如何发挥作用的，还尚不清楚。因此需要研发一种在复杂介质环境中对一氧化碳能高选择性识别的测定方法。尽管已经开发出许多用于CO成像的有机荧光探针，但是这些探针在紫外或可见光范围内激发，具有穿透深度浅，毒性大等缺点，这限制了它们在生物系统中的应用。 本文首次提出了一种新的策略来构建基于UCNPs的UCL传感CO纳米系统。 基于LRET机理，用花菁染料修饰镧系元素掺杂的上转换纳米颗粒（UCNPs），通过NIR激发的比率荧光光谱法显示了对CO的快速响应，具有高灵敏度和高稳定性的优点。

关键词：一氧化碳 花菁染料 上转换纳米粒子 荧光探针

Cyanine dye modified up-conversion nanometer carbon monoxide probe

Abstract

Carbon monoxide (CO) is considered to be the second gaseous transmitter involved in a series of physiological and pathological processes. If excessive intake of exogenous carbon monoxide can lead to carbon monoxide poisoning in biological organisms, carbon monoxide has long been considered to be only a toxic and harmful substance. Physiological effects have long been ignored by people. Therefore, it is necessary to develop a method for highly selective identification and determination of carbon monoxide in a complex medium environment. Although many organic fluorescent probes have been developed for CO imaging, the excitation of these probes were located in the ultraviolet or visible range, have the disadvantages of shallow penetration depth, high toxicity, etc., which limits their application in biological systems. This paper presents for the first time a new strategy to construct a UCL sensing CO nanosystem based on UCNPs. Based on the LRET mechanism, upconversion nanoparticles doped with lanthanides, modified UCNPs with cyanine dyes, and NIR-excited ratiometric fluorescence spectroscopy showed rapid response to CO, with the advantages of high sensitivity and high stability.

Keywords: carbon monoxide；cyanine dye；upconversion nanoparticles；fluorescent probe

目录

摘 要…………………………………………………………………………Ⅰ

ABSTRAC…………………………………………………………………………Ⅱ

第一章 综述………………………………………………………………………1

1.1引言…………………………………………………………………………1

1.2上转换纳米材料……………………………………………………………2

1.3 CO的传统检测方法……………………………………………………2

1.4荧光探针分析法……………………………………………………………2

1.5 CO荧光探针……………………………………………………………4

1.6本论文的研究工作内容……………………………………………………5

第二章 基于CO的花菁染料修饰稀土纳米晶上转换效应进行高效检测的荧光探针合成与性质研究…………………………6

2.1 实验部分…………………………………………………………………6

2.1.1 实验使用仪器与试剂… ………… …………………………………6

2.1.2 中间体的合成…………………… ………………………… ………7

2.2 结果与讨论………………………………… ……………………………10

2.2.1 CyD1-UCNPs @ mSiO₂的制备与表征… …………………… ……10

2.2.2纳米系统CyD1-UCNPs@mSiO₂ PdCl₂用于CO检测的原理………… …… … ………… …… ………… …… ……………11

2.2.3纳米系统CyD1-UCNPs @ mSiO₂ PdCl₂对CO的紫外-可见滴定光谱性质的研究…………………… ……… ……………………… …12

2.2.4纳米系统CyD1-UCNPs @ mSiO₂ PdCl₂对CO荧光光谱性质的研究………… ………………… ……………………… ……………13

2.2.5 纳米系统CyD1-UCNPs @ mSiO₂ PdCl₂对CO的特异性检测……………………… ……………… …………… ……………14

2.3 本章小结……………………………………………………………………15

第三章 结论与展望 ………………………………………… …………………16

3.1 结论…………………………………………………………………………16

3.2 展望…………………………………………………………………………16

参考文献……………………………………………………………………………17

附 录……………………………………………………………………………20

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