本研究旨在製備一非侵入式唾液葡萄糖感測電極。近年來，由於人類飲食習慣、生活作息的改變，使糖尿病患者日益增加，然而目前量測血糖方式仍以扎針採血為主，為因應患者人口數增加的趨勢以及減緩病患量測血糖的不便，研發非侵入式感測電極有其必要性。利用奈米碳材料-奈米金顆粒修飾FTO電極，配合注入葡萄糖氧化酶於系統中，期望提升葡萄糖感測電極的敏感度、量測範圍以及專一性，以利其具備實際應用之潛力。
實驗分別利用滴鑄法與直接成長法製備三種複合修飾電極，搭配使用材料分析儀器探討不同電極之表面形貌與微結構差異，並以電化學方法分析各電極之電化學性質，接著利用檢測系統中氧氣的消耗量作為葡萄糖感測機制來探討電極結構、電化學性質與感測結果之相互關係與影響。研究結果顯示，隨著電極的電子轉移阻抗降低，其敏感度會上升，然而感測線性範圍則會受電極表面形貌與電極結構的交互影響。本實驗以直接成長法製備電極(Au-gCNTs/FTO)表現出最高的敏感度，達213.59 μA/mMcm2，以滴鑄法製備電極(AuCNTs/FTO、5% rGO/AuCNTs/FTO)表現出較大之線性感測範圍：20 – 700 μM，雖然表現的優勢不盡相同，但三種電極皆顯示出偵測葡萄糖的高度能力，且具較大線性範圍的滴鑄法製備電極更顯示其實際應用於診斷糖尿病患者之潛力。

The study aimed to fabricate a noninvasive saliva glucose sensor. Due to changes in human dietary habits and lifestyle, people with diabetes continuously increase recently. However, most blood glucose measurement involves invasive and painful sampling procedure, and therefore, to alleviate the inconvenience of the patients, the development of non-invasive sensing electrodes is necessary. With the synergistic effects of carbon nanomaterials-gold nanoparticles composite modified FTO electrode and the glucose oxidase enzyme, the improvement of sensitivity, sensing linear range, and selectivity of the sensing electrode can be expected and equipped the electrode with the potential of practical application.
In this work, three modified electrodes were respectively fabricated with drop-casting method and direct-growing method. The morphology and microstructure of electrodes were studied by SEM, TEM and XRD, while their electrochemical properties were investigated by electrochemical methods including cyclic voltammetry and EIS. Finally, the glucose sensing tests were performed and the relation between each property was discussed. The results of electrode show negative relationship between electron transfer resistance and the sensitivity; however, the sensing linear range was also influenced by the morphology and the structure of electrode. Since Au-gCNTs/FTO, fabricated with direct-growing method, exhibited the best sensitivity of 213.59 μA/mMcm2, the drop-casting modified electrode, including AuCNTs/FTO and 5% rGO/AuCNTs/FTO, show wider sensing linear range of 20 – 700 μM glucose concentration. Despite different advantages of each electrode, all electrodes present high potential for diabetic diagnosis and practical application.

摘要 I
Abstract II
致謝 III
目次 IV
表目次 VII
圖目次 VIII
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 糖尿病與市售血糖檢測方法 3
2.1.1 糖尿病類型與病徵 3
2.1.2 市售血糖檢測方法 5
2.1.3 唾液葡萄糖濃度及檢測 5
2.2 葡萄糖感測機制 7
2.2.1 酵素型葡萄糖感測 7
2.2.1.1 第一世代葡萄糖感測電極原理 8
2.2.1.2 第二世代葡萄糖感測電極原理 9
2.2.1.3 第三世代葡萄糖感測電極原理 10
2.2.2 第四代非酵素型葡萄糖感測 11
2.3 奈米材料修飾電極在葡萄糖感測器上之應用 12
2.3.1 奈米碳材料修飾電極 12
2.3.2 奈米金屬粒子修飾電極 13
2.3.3 導電高分子修飾電極 14
2.4 葡萄糖感測器之基材選用 16
2.4.1 玻璃碳電極基材 16
2.4.2 貴金屬電極基材 17
2.4.3 導電玻璃基材 18
2.5 本實驗室過去於生醫感測的回顧 19
第三章 實驗方法 27
3.1 實驗藥品 27
3.2 實驗製程設備 27
3.3 實驗製備流程 29
3.3.1 滴鑄法之複合電極製備 29
3.3.1.1 氟摻雜氧化錫玻璃基板之前處理 29
3.3.1.2 聚苯胺之合成 30
3.3.1.3 奈米碳管之酸處理 30
3.3.1.4 奈米金粒子之合成 31
3.3.1.5 還原氧化石磨烯之製備 32
3.3.1.6 電極修飾之滴鑄方法 32
3.3.2 直接成長法之複合電極製備 33
3.3.2.1 氟摻雜氧化錫玻璃基板之前處理 33
3.3.2.2 奈米碳管之成長 33
3.3.2.3 奈米金粒子之合成 34
3.4 分析技術與設備 34
3.4.1 葡萄糖感測電極之材料性質分析 34
3.4.1.1 場發射掃描式電子顯微鏡 35
3.4.1.2 場發射掃描穿透式球差修正電子顯微鏡 35
3.4.1.3 X光繞射儀 36
3.4.2 葡萄糖感測電極之操作步驟及電化學性質分析 37
3.4.2.1 葡萄糖感測裝置之架設 37
3.4.2.2 葡萄糖與酵素濃度配置 37
3.4.2.3 實測唾液處理 38
3.4.2.4 循環伏安法測試分析 38
3.4.2.5 電化學阻抗頻譜測試分析 39
3.4.2.6 電極反應表現定義 39
第四章 結果與討論 46
4.1 滴鑄法 － AuCNTs (10 L)/FTO電極之設計與製備 46
4.1.1 奈米金顆粒還原時間之影響 46
4.1.2 滴鑄層數之影響 48
4.2 滴鑄法 － 5% rGO (1 L)/AuCNTs (9 L)/FTO電極之設計與製備 49
4.2.1 還原氧化石墨烯比例之影響 50
4.3 直接成長法 － AuNPs-gCNTs複合電極之分析 51
4.3.1 電極結構之分析 51
4.4 不同複合電極設計之電化學效能分析比較 53
4.4.1 葡萄糖感測電極之形貌分析 53
4.4.2 循環伏安法分析 54
4.4.3 電化學阻抗頻譜測試分析 55
4.5 不同複合電極設計之感測效能分析比較 56
4.5.1 葡萄糖感測機制 57
4.5.2 葡萄糖感測效能分析 58
4.5.3 干擾物測試分析 60
4.5.4 唾液實測分析 61
第五章 結論 85
參考文獻 87

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