本文聚焦於非侵入式唾液葡萄糖感測之研究，因應近年人類生活習慣、飲食風格的改變，現今全球糖尿病患者呈現逐漸增加的趨勢，另外當前扎針採血量測血糖對於病患及潛在病患造成不便，因此降低感測裝置量測時的不適感進而提升大眾對於量測的接受度，非侵入式感測裝置因而引發熱門的研究。本文將結合奈米碳管(Carbon nanotubes, CNTs)以及導電高分子聚吡咯(Polypyrrole, PPy)修飾氟摻雜氧化錫導電玻璃基板(Fluorine-doped tin oxide, FTO)，並搭配葡萄糖氧化酶的使用以期製備出具有高靈敏度、高感測濃度範圍以及高度專一性之電極。
實驗使用化學聚合法沉積導電高分子polypyrrole於FTO基板(PPy/FTO)，並利用滴鑄法修飾奈米碳材料於導電玻璃表面(acid-CNTs/PPy/FTO)，搭配不同材料分析儀器探討不同修飾程度之電極表面形貌及微結構變化，使用電化學法之三電極系統分析電化學表現，隨後利用此檢測系統搭配葡萄糖氧化酶進行葡萄糖感測之研究。綜合材料分析、電化學表現及感測結果研究其關聯性。根據研究結果，隨著FTO基板經過不同材料的修飾後，其電子阻抗隨之降低，能夠有效提升其靈敏度。本實驗比較不同電極尺寸大小與不同奈米碳管酸處理時間對電極感測效能的影響，感測結果顯示2.5小時酸處理修飾電極具有最優異的感測表現，高靈敏度95.26 μA/mMcm2、線性區間10 – 700 μM，能夠在正常人及潛在病患的唾液葡萄糖的濃度中展現出優異線性表現，顯示此電極在唾液葡萄糖感測之發展潛力。

The work focuses on the study of noninvasive saliva glucose sensor. Recently, the diabetics continuously increase all over the world, which is caused by the change in human daily life. Nowadays, the sampling process through lancet for patients is an invasive method which causes pain and discomfort for human body. In order to alleviate the inconvenience for diabetics and those who are potentially at high risk of illness, the research for noninvasive sensing device is imperative. Combining the excellent electrochemical properties of carbon nanomaterials modified on conductive polymer, and glucose oxidase enzyme with high selectivity, we expect to fabricate an outstanding electrodes with high sensitivity and wide linear sensing range.
This study uses chemical polymerization method to deposit polypyrrole on fluorine-doped tin oxide conductive glass (FTO) substrate, and then modifies the electrode with carbon nanotubes (CNTs) by drop-casting method. The sensing electrodes are studied through SEM and TEM to investigate the morphology and microstructure, while electrochemical properties and glucose sensing test are performed by a three-electrodes system, including cyclic voltammetry and EIS test. The results show that with the modification layer by layer, the electron transfer resistance decreases, and the sensing performance is influenced by the size of electrodes and acid treatment time of CNTs. The sensing result shows that the CNTs, acid-treated for 2.5 hours, modified electrodes exhibit best sensing performance, with high sensitivity of 95.26 μA/mMcm2,wider linear range of 10 – 700 μM and high linearity of R2 value 0.9958. Based on the glucose sensing result, all electrodes present high potential toward noninvasive saliva glucose sensor for diabetic diagnosis.

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 糖尿病介紹 3
2.1.1 糖尿病種類 4
2.1.2 糖尿病檢測方法 5
2.1.3 唾液葡萄糖濃度及檢測 8
2.2 葡萄糖感測電極發展及機制 11
2.2.1 葡萄糖之光學感測法 12
2.2.2 葡萄糖之電化學感測法 12
2.2.3 葡萄糖之感測機制 13
2.2.3.1 第一世代葡萄糖感測器 14
2.2.3.2 第二世代葡萄糖感測器 14
2.2.3.3 第三世代葡萄糖感測器 16
2.2.3.4 第四世代葡萄糖感測器 18
2.3 奈米材料於葡萄糖感測之應用 19
2.3.1 奈米碳材料修飾電極 19
2.3.2 導電高分子修飾電極 22
2.4 葡萄糖感測電極之基材選擇 24
2.4.1 玻璃碳電極基材 24
2.4.1 金屬電極基材 27
2.4.2 導電玻璃基材 27
2.5 本實驗室於生醫感測領域之回顧 29
2.5.1 多巴胺感測 29
2.5.2 葡萄糖感測 29
第三章 實驗方法 31
3.1 實驗藥品 32
3.2 實驗製程設備 34
3.3 實驗製備流程 35
3.3.1 滴鑄法之電極製備 35
3.3.1.1 氟摻雜氧化錫玻璃基板之前處理 35
3.3.1.2 聚吡咯之合成 36
3.3.1.3 奈米碳管之酸處理 37
3.3.1.4 電極修飾之滴鑄方法 38
3.4 電極之材料分析及電化學感測效能 38
3.4.1 感測電極之材料分析 38
3.4.1.1 冷場發射掃描式電子顯微鏡 39
3.4.1.2 拉曼光譜儀 39
3.4.1.3 X射線光電子能譜儀 40
3.4.1.4 穿透式電子顯微鏡 40
3.4.1.5 原子力顯微鏡 41
3.4.1.6 流變儀 41
3.4.2 感測電極之電化學分析 42
3.4.2.1 三電極系統介紹 42
3.4.2.2 循環伏安法及阻抗測試頻譜分析 44
3.4.2.3 實驗待測液之配置 45
3.4.2.4 電極反應表現定義 47
第四章 結果與討論 48
4.1 化學法聚合聚吡咯於導電玻璃之影響分析 48
4.1.1 冷場發射掃描式電子顯微鏡 48
4.1.2 不同沉積時間之聚吡咯循環伏安圖分析 50
4.1.3 X射線光電子能譜儀 52
4.2 奈米碳管/聚吡咯/導電玻璃複合電極之特性分析 54
4.2.1 拉曼能譜儀 54
4.2.2 穿透式電子顯微鏡 55
4.2.3 冷場發射掃描式電子顯微鏡 57
4.2.4 不同碳管修飾層數之電化學性質分析 59
4.2.5 不同複合電極之電化學性質分析 62
4.2.6 原子力顯微鏡 64
4.2.7 電極之電化學反應探討 66
4.3 奈米碳管/聚吡咯/導電玻璃複合電極感測效能探討 69
4.3.1 葡萄糖感測機制 69
4.3.2 電極尺寸對於葡萄糖感測之影響 70
4.3.3 不同酸處理時間之碳管修飾電極對感測之影響 77
4.3.4 感測電極之酵素親和力探討 84
4.3.5 模擬唾液感測效能分析 85
4.3.6 電極之干擾性測試 90
4.3.7 電極之再現性與穩定性表現探討 92
第五章 結論 94
參考文獻 96

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