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研究生: 劉侑昂
Yu-Ang Liu
論文名稱: 樹狀奈米金與rGO複合材料合成與其電化學感測之研究
Synthesis of Gold Nanodendrites-Reduced Graphene Oxide Composite Materials for Electrochemical Analysis
指導教授: 洪偉修
Hung, Wei-Hsiu
學位類別: 碩士
Master
系所名稱: 化學系
Department of Chemistry
論文出版年: 2014
畢業學年度: 102
語文別: 中文
論文頁數: 87
中文關鍵詞: 電化學還原氧化石墨烯樹狀金電極血紅蛋白葡萄糖氧化酶生物感測器
英文關鍵詞: electrochemically reduced graphene oxide, gold dendrite, hemoglobin, glucose oxidase, biosensor
論文種類: 學術論文
相關次數: 點閱:150下載:5
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  • 本研究利用葡萄糖氧化酶(GOx)和血紅蛋白(Hb)兩種酵素分別偵測葡萄糖與過氧化氫,本實驗製作了還原態氧化石墨烯(rGO)與樹狀金電極(GD)的複合材料(GD/rGO)並搭配酵素的薄膜修飾進而製備高靈敏度之生物感測器。應用循環伏安技術和計時電流安培法研究此電極電化學特性。由電化學阻抗(EIS)分析酵素已成功修飾,在X射線光電子能譜(XPS)及拉曼散射光譜的鑑定下證實氧化石墨烯已完成電化學法還原並與樹狀金電極形成複合材料。並利用掃描電子顯微鏡觀察薄膜的表面型態。且根據電化學實驗計算出酵素與修飾薄膜電極表面具快速的電子轉移能力。
    從計時安培法結果顯示此GD/rGO/GOx/Nf(Nafion)薄膜對於葡萄糖偵測展現出<3 s的電流響應時間,並具有0.008 mM到7.2 mM寬廣的偵測線性範圍、5 µM最小偵測極限和良好的靈敏度25.23 µAmM-1cm-2。另一方面,GD/rGO/Hb/Nf薄膜偵測過氧化氫也有<5 s的電流響應時間,寬廣的線性範圍0.003 mM到22.7 mM、與極低的偵測極限1 µM和0.623 mAmM-1cm-2的靈敏度。
    GOx薄膜修飾電極在含有電子傳導媒介偵測葡萄糖時展現出好的電催化活性,而Hb對於偵測過氧化氫也有卓越的電催化還原能力,並且在製備過程中具備簡易、有效率及無環境污染等優點。

    In this thesis, we report the fabrication two highly sensitive hydrogen peroxide and glucose biosensor based on immobilization of glucose oxidase (GOx) and hemoglobin (Hb) on the composites of graphene oxide (rGO) gold dendrites (GD), which are electrodeposited on the GC electrode (GCE). The electrochemical characteristics of the biosensor were studied by cyclic voltammetry (CV) and amperometry. The modified process was characterized by electrochemical impedance spectroscopy (EIS) and cyclic votammetry. The morphologies of modified film were investigated with scanning electron microscopy (SEM) and the element of film was investigated with X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. GOx and Hb were well immobilized onto the GD/rGO film on the rGO and GD composites. The experimental data demonstrate faster electron transfer between enzymes and the modified electrode surface.
    The results of amperometry response indicates that GD/rGO/GOx/Nf(Nafion) film displayed a fast response of less than 3 s and exhibits low detection limit of 5 µM with wide linear range of 0.008-7.2 mM and good sensitivity of 25.23 µAmM-1cm-2 for glucose detection. On the other hand, the GD/rGO/Hb/Nf film also displays a response of less than 5 s. The proposed hydrogen peroxide biosensor shows a low detection limit of 1 µM with linear range of 0.003-22.7 mM and exhibits excellent sensitivity of 0.623 mAmM-1cm-2.
    The modified films show high electrocatalytic activity towards glucose in the presence of mediator and exhibit a remarkable electrocatalytic activity for the reduction of hydrogen peroxide. Moreover the fabrication of these two biosensors was simple, efficient and green technique.

    摘要 I Abstract III 謝誌 V 目錄 VI 圖目錄 VIII 表目錄 XI 第一章 緒論 1 1.1感測器介紹 1 1.2化學感測器 3 1.3生物感測器 6 1.4電化學生物感測器技術 7 1.5電化學分析法 9 1.6化學修飾電極 10 1.7石墨烯 11 1.8氧化石墨烯與還原態氧化石墨烯 13 1.9脈衝式電流電化學沉積法 16 1.10三維樹狀金電極 17 第二章 儀器與實驗藥品 19 2.1儀器介紹 19 2.1.1 X-ray光電子能譜儀(X-ray photoelectron spectroscopy, XPS) 19 2.1.2循環伏安法(Cyclic Voltammetry, CV) 23 2.1.3電化學交流阻抗(electrochemical impedance spectroscopy, EIS) 25 2.1.4安培法(Amperometric, i-t curve) 27 2.1.5拉曼光譜(Raman spectrum) 28 2.1.6掃瞄式電子顯微鏡(Scanning Electron Microscopy, SEM) 32 2.1.7能量散射光譜儀(Energy Dispersive System, EDS) 34 2.2實驗藥品 36 2.3實驗步驟 37 第三章 葡萄糖生物感測器 39 3.1 前言 39 3.2葡萄糖氧化酶簡介 40 3.3葡萄糖生物感測機制 41 3.4結果與討論 43 3.4.1氧化石墨烯之電化學還原(rGO) 43 3.4.2還原態氧化石墨烯-樹狀金複合材料(GD/rGO)結構鑑定 44 3.4.3 GD/rGO/GOx修飾電極的電化學阻抗分析 49 3.4.4 GD/rGO/GOx/Nf薄膜修飾電極對pH值及掃描速率之研究 51 3.4.5薄膜修飾電極利用氧氣消耗以電化學循環伏安法偵測葡萄糖 55 3.4.6薄膜修飾電極利用電子傳導媒介(Mediator)以電化學循環伏安法偵測葡萄糖 56 3.4.7薄膜修飾電極以計時安培法偵測葡萄糖 59 第四章 血紅蛋白酵素電極偵測過氧化氫 64 4.1前言 64 4.2血紅蛋白介紹 65 4.3酵素催化還原過氧化氫 66 4.4結果與討論 67 4.4.1 GD/rGO/Hb/Nf薄膜修飾電極表面型態與元素分析 67 4.4.2 GCE/GD/rGO/Hb修飾電極的電化學阻抗分析 69 4.4.3 GD/rGO/Hb/Nf薄膜修飾電極對pH值及掃描速率之研究 70 4.4.4薄膜修飾電極以電化學循環伏安法偵測過氧化氫 73 4.4.5薄膜修飾電極以計時安培法偵測葡萄糖 75 第五章 結論 79 第六章 參考文獻 80

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