臺灣博碩士論文加值系統

本篇論文利用修飾不同分子的功能性金奈米粒子（Gold nanoparticles﹐AuNPs），藉由AuNPs本身具有高消光係數（Extinction coefficient）和特殊光學性質，開發出活性氧化物（Reactive oxygen species﹐ROS）與重金屬離子感測器。
一、以修飾異硫氰酸螢光素之金奈米粒子作為活性氧化物感測器—應用於血糖之偵測：本篇研究當中，我們利用修飾異硫氰酸螢光素之金奈米粒子（Fluorescein isothiocyanate-gold nanoparticles﹐FITC-AuNPs），可以簡單且靈敏地偵測ROS。當FITC螢光分子吸附在AuNPs表面，因為螢光共振轉移（Fluorescence resonance energy transfer﹐FRET）的原理，FITC分子的螢光訊號大部分都被AuNPs抑制。若我們把2-硫基乙醇（2-Mercaptoethanol﹐2-ME）加入到FITC-AuNPs中，原本吸附在AuNPs表面的FITC分子會被取代出來，而釋放到溶液中，使得螢光強度明顯增加。較為關鍵的是ROS可將兩個2-ME氧化成一個含雙硫鍵（Disulfide bond）的分子，而形成雙硫鍵的結構將無法取代出FITC分子，因此螢光訊號仍被抑制。綜合上述結果，當ROS含量越多，形成含有雙硫鍵的分子越多，而偵測到的螢光訊號相對越低，故可作為ROS感測器。對分析物ROS之最低可偵測濃度（Minimum detectable concentration﹐MDC）分別為：H2O2，1000 nM；超氧陰離子（Superoxide anion），600 nM；氫氧自由基（Hydroxyl radical）。基於此概念，我們開發出一套兩步驟的葡萄糖（Glucose）偵測法：首先，Glucose與其氧化酶（Glucose oxidase﹐GOx）進行反應將產生過氧化氫（Hydrogen peroxide﹐H2O2）；接著，將所產生之H2O2與2-ME反應，再透過前面的方法，使用FITC-AuNPs進行偵測，對於Glucose之MDC為1000 nM。藉由本偵測系統亦成功偵測到血清中的Glucose。
二、利用修飾Tween 20界面活性劑之檸檬酸鈉金奈米粒子作為汞離子和銀離子感測器：在第二部分實驗中，我們利用修飾Tween 20界面活性劑之檸檬酸鈉金奈米粒子（Tween 20-citrate-gold nanoparticles﹐Tween 20-citrate-AuNPs），發展出一套快速且具有高選擇性的感測器，可以應用於定量分析Hg2+和Ag+。我們由實驗中發現，檸檬酸鈉包覆的金奈米粒子（Citrate-gold nanoparticles﹐Citrate-AuNPs）修飾上Tween 20界面活性劑，Tween 20分子只是穩固覆蓋在檸檬酸鈉分子上，並未將檸檬酸鈉取代出來。而使用Tween 20界面活性劑主要是保護Citrate-AuNPs可以穩定存在高離子強度溶液中，至於檸檬酸鈉分子是扮演還原劑角色，可將Hg2+或Ag+還原並於AuNPs表面形成金-汞合金（Au-Hg Alloys）或銀殼層（Ag Shell），導致Tween 20分子被迫脫離奈米粒子表面，如此AuNPs無法繼續穩定存在高離子強度溶液中而變為聚集狀態。本篇開發Tween 20-citrate-AuNPs感測器，使用氯化鈉（NaCl）和乙烯二胺四乙酸（Ethylenediaminetetraacetic acid﹐EDTA）分別作為偵測Hg2+和Ag+的遮蔽試劑（Masking agents），其MDC均可達100 nM。此外，使用本系統亦可偵測銀奈米粒子（Silver nanoparticles﹐AgNPs），其MDC為1 pM。據我們所知，本研究為首次利用同一種探針（Tween 20-citrate-AuNPs）即可同時偵測Hg2+和Ag+，並成功透過此系統分析飲用水中Hg2+、Ag+ 和AgNPs，以及海水中Hg2+。

摘要I
目錄IV
圖表目錄VII
縮寫表X

第一章 以修飾異硫氰酸螢光素之金奈米粒子作為活性氧化物感測器—應用於血糖之偵測
一、前言1
二、實驗部分9
2.1、藥品與溶液配製9
2.2、儀器裝置11
2.3、FITC-AuNPs之合成方法13
2.4、ROS和Glucose之配製14
2.5、真實樣品之處理與配製15
三、結果與討論16
3.1、透過抑制螢光之概念偵測H2O216
3.2、探討反應中H2O2與2-ME之莫耳數比23
3.3、FITC-AuNPs對ROS和Glucose進行偵測26
3.4、以FITC-AuNPs偵測血清中Glucose32
四、結論34
五、參考文獻35

第二章 利用修飾Tween 20界面活性劑之檸檬酸鈉金奈米粒子作為汞離子和銀離子感測器
一、前言43
二、實驗部分49
2.1、藥品與溶液配製49
2.2、儀器裝置51
2.3、奈米粒子之合成53
2.4、樣品配製55
2.5、真實樣品之偵測56
三、結果與討論57
3.1、偵測機制之探討57
3.2、證明Au-Hg Alloys和Ag Shell之生成59
3.3、研究Surfactant長度、奈米粒子濃度與離子強度66
3.4、Tween 20-citrate-AuNPs對Hg2+和Ag+之選擇性探討71
3.5、Tween 20-citrate-AuNPs對Hg2+和Ag+之靈敏度探討及真實樣品的應用75
四、結論84
五、參考文獻85

第一章以修飾異硫氰酸螢光素之金奈米粒子作為活性氧化物感測器—應用於血糖之偵測
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第二章利用修飾Tween 20界面活性劑之檸檬酸鈉金奈米粒子作為汞離子和銀離子感測器
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