隨著經濟之成長，人們生活作息與飲食隨之產生巨大改變，雖近年來對於血糖控管意識提升，卻礙於現今血糖檢測尚存有缺點，使得人們難以主動執行血糖監控，因此全球糖尿病之患者數仍持續快速攀升。故本研究之目的為研發一電極用於唾液葡萄糖之感測，以提高非侵入之形式，提供更方便的檢測方法，期望提高世人對健康控管意願，並改善量測血糖之不便。
本研究利用化學氣相沉積法直接成長奈米碳管於FTO導電玻璃上，並藉由修飾聚乙烯亞胺高分子，使得葡萄糖氧化酶以靜電力作用吸附於碳管表面，製備出具有高敏感度及高專一性之電極。搭配各式分析儀器探討電極之形貌與結構之差異，並以電化學方法探討電極之電子傳遞能力，最後，藉由循環伏安法分析法偵測系統中氧氣之消耗量以及葡萄糖氧化酶氧化還原反應所產生電流差作為葡萄糖感測機制。研究結果顯示，經由成長的奈米碳管可以大幅提升電極之電子傳遞能力，且其網狀結構能夠提供電極高粗糙表面，搭配聚乙烯亞胺高分子作為碳管與酵素之間的媒介，使得葡萄糖氧化酶可以有效的被固定於電極之上，而展現優良的感測效果，其中電極之氧氣還原峰敏感度可以達64 μA/μMcm2，且線性範圍涵蓋50-700 μM葡萄糖濃度，顯示出其具有應用於測量唾液葡萄糖濃度之潛力。

Although the awareness of body glucose management has arose in recent years, few people exactly execute monitoring for blood glucose level due to the discomfort when using blood glucose meter, which caused the number of diabetics keep increasing sharply. In order to increase the willingness of testing of glucose level and further provide a better life quality for diabetics, the aim of this research is to develop an electrode for non-invasive glucose sensor by measuring glucose level in saliva. In this work, carbon nanotubes (CNTs) are fabricated onto fluorine doped tin oxide (FTO) substrate by using the chemical vapor deposition method, then polyethylenimine (PEI) and glucose oxidase (GOx) are immobilized on CNTs surface by the drop casting method. To further investigate the morphology and microstructure of the electrode, SEM, TEM, Raman, XRD, and AFM are used, while the electrochemical properties and sensing performance are studied by the electrochemical methods including EIS and cyclic voltammetry (CV). According to the results, the CNTs, directly growing on the FTO substrate can greatly enhance the charge transfer ability, and with the network structure of CNTs forest, it can provide a rougher surface for PEI and GOx to be stably immobilized, so that both oxygen reduce reaction and enzyme redox reaction can be detected by the CV method, and the current difference in CV tests of the fabricated electrode can be used as the signal for glucose sensing. Finally, the FTO-CNTs/PEI/GOx electrode exhibits the best sensitivity of 64 µA/mMcm2 with a wide linear range from 50 to 700 µM glucose concentration, which possesses high potential for practical application.

摘要 I
Abstract II
致謝 III
目次 IV
表目次 VII
圖目次 IX
第一章 緒論 1
1.1 前言 1
1.2 研究動機 2
第二章 文獻回顧 3
2.1 糖尿病與診斷方法 3
2.1.1 糖尿病類型和病徵 4
2.1.2 糖尿病診斷及檢測方法 5
2.1.3 唾液葡萄糖濃度範圍 6
2.2 葡萄糖感測系統發展 9
2.2.1 酵素型葡萄糖感測系統 10
2.2.1.1 第一世代葡萄糖感測原理 12
2.2.1.2 第二世代葡萄糖感測原理 13
2.2.1.3 第三世代葡萄糖感測原理 14
2.2.2 非酵素型葡萄感測系統 15
2.3 奈米碳管之介紹 17
2.3.1 奈米碳管製備方法 17
2.3.2 奈米碳管結構與特性 19
2.3.3 奈米碳管於葡萄糖感測器之應用 20
2.4 本實驗室過去於葡萄糖感測之回顧 23
第三章 實驗方法 24
3.1 實驗藥品及製程儀器 24
3.2 電極製備流程 28
3.2.1 摻氟氧化錫玻璃前處理 29
3.2.2 濺鍍法沉積鎳金屬於基板 29
3.2.3 以化學氣相沉積法成長奈米碳管於基板 30
3.2.4 聚乙烯亞胺之修飾 30
3.2.5 葡萄糖氧化酶之修飾 31
3.3 實驗分析儀器與技術 32
3.3.1 電極之材料性質分析 32
3.3.1.1 場發射式掃描電子顯微鏡 32
3.3.1.2 X光繞射分析儀 33
3.3.1.3 拉曼光譜儀 34
3.3.1.4 聚焦離子束 34
3.3.1.5 場發射掃描穿透式球差修正電子顯微鏡 35
3.3.1.6 原子力顯微鏡 36
3.3.2 電極之電化學性質分析及葡萄糖感測 36
3.3.2.1 電化學感測裝置 36
3.3.2.2 葡萄糖濃度配置與感測操作 37
3.3.2.3 循環伏安法測試 38
3.3.2.4 電化學阻抗頻譜測試 39
3.3.2.5 電極感測表現定義 39
第四章 結果與討論 41
4.1 以化學氣相沉積法成長奈米碳管 41
4.1.1 溫度條件之影響 42
4.1.2 乙炔流量之影響 45
4.1.3 奈米碳管成長機制探討 47
4.2 電極之結構與電化學分析 51
4.2.1 鎳含量對FTO-CNTs之電化學影響 51
4.2.1.1 SEM表面形貌分析 51
4.2.1.2 循環伏安法分析 55
4.2.1.3 阻抗頻譜測試分析 56
4.2.2 電極之酵素修飾與電化學分析 59
4.2.2.1 奈米碳管對酵素修飾之影響 59
4.2.2.2 聚乙烯亞胺對酵素修飾之影響 61
4.2.2.3 阻抗頻譜測試分析 63
4.2.3 電極於磷酸鹽緩衝溶液中之電化學行為 65
4.2.3.1 掃速探討 65
4.2.3.2 酸鹼度探討 66
4.3 電極之葡萄糖感測機制和效能探討 69
4.3.1 葡萄糖感測機制探討 69
4.3.2 電位窗對感測之影響 72
4.3.3 葡萄糖感測之效能 74
4.3.4 干擾物測試 89
4.3.5 人工唾液葡萄糖感測 91
4.3.6 再現性與穩定性測試 94
第五章 結論 96
參考文獻 98

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