臺灣博碩士論文加值系統

本論文主要是探討利用導電奈米鑽石當作工作電極，再利用氧化銅、氫氧化鎳做修飾，最後再利用不同結構的基板來製作葡萄糖感測器，探討從結構及材料種類及材料厚度來實驗出最佳的葡萄糖感測器條件，本論文利用MPCVD沉積摻雜氮的導電奈米鑽石薄膜當做工作電極，利用濺鍍設備濺鍍金屬鎳及氧化銅，再利用循環伏安法使金屬鎳改質成氫氧化鎳，最後進行元件的物性及葡萄糖靈敏度量測，其結果為有加金字塔結構的靈敏度相對較高，在氫氧化鎳部分，氫氧化鎳(100nm)厚度濺鍍於金字塔結構鑽石薄膜的靈敏度有最高的值3070(μA mM −1 cm −2)，而在氧化銅的部分，氧化銅(75nm)厚度濺鍍於金字塔結構鑽石薄膜的靈敏度有最高的值1993(μA mM −1 cm −2)，而就穩定性分析來說，氧化銅的試片平均在元件放置28天後只衰減不到其靈敏度的10%，但氫氧化鎳的試片平均在元件放置28天後衰減其靈敏度的36%，可見氧化銅比氫氧化鎳有更好的穩定性，其中導電鑽石薄膜提供良好的葡萄糖傳感特性，對於未來生物感測之應用具有一定的潛力。

We have designed glucose sensors based on the use of highly conducting nitrogen incorporated diamond film (NDFs) electrodes grown by microwave plasma enhanced chemical vapor deposition. The post deposition of Ni(OH)2 and CuO on Pyramidal NDFs and plane NDFs, which reveal differences for the glucose detection. The systematic cyclic voltammetry measurements on the 100nm thickness of Ni(OH)2 on the pyramidal NDFs glucose sensors attains higher sensitivity properties(3070(μA mM-1 cm-2)) than those of Ni(OH)2(120nm)/plane NDFs(2444(μA mM-1 cm-2)) and CuO(75nm)/pyramid NDFs glucose sensors(1993(μA mM-1 cm-2)).
In terms of stability, CuO/NDFs based sensors reveals much better stability than Ni(OH)2/NDFs based sensors. The CuO/NDFs test chips were decreased less than 10% however, Ni(OH)2/NDFs based sensors were decreased up to 36% after exposing in air at room temperature for 28 days.
The higher sensitivity with high selectivity and reliable stability might be due to the use of the highly electrically conductive diamond film electrodes, which is responsible for good glucose sensing properties, and exhibits a significant degree of potential on the future bio-sensing applications.

目 錄
中文摘要 Ⅰ
英文摘要 Ⅱ
誌謝 III
目錄 IV
圖目錄 VIII
表目錄 XVIII
第一章　緒論 1
1.1 前言 1
1.2 研究動機 3
第二章　文獻回顧 5
2.1 感測器 5
2.2 生物感測器 6
2.3 葡萄糖感測器 10
2.3.1 葡萄糖感測器的起始 10
2.3.2 葡萄糖感測器發展世代 11
2.3.3 葡萄糖檢測方法 14
2.3.4 非酵素型葡萄糖感測器 14
2.3.4.a 非酵素型葡萄糖感測器電極種類 15
2.3.4.b 非酵素型葡萄糖感測器修飾物種類 15
2.4 葡萄糖結構與性質 16
2.4.1 葡萄糖 16
2.4.2 葡萄酸內酯 17
2.4.3 葡萄糖酸 18
2.5 奈米鑽石 19
2.5.1 奈米鑽石薄膜特性簡介 19
2.5.2 奈米鑽石成核機制 21
2.5.3 奈米鑽石薄膜之成長方法 23
2.6 電化學分析法 27
2.6.1 電化學分析法-三電極系統 27
2.6.2 電化學分析法-循環伏安法 28
2.6.3 電化學分析法-定電位沈積分析法 29
2.6.4 電化學分析法-定電流沈積分析法 30
2.7 矽基板金字塔結構之蝕刻機制 30
第三章　實驗方法 33
3.1 實驗流程 33
3.2 矽基板金字塔結構之製備 34
3.2.1 矽晶圓清洗處理流程 34
3.2.2 鹼性蝕刻溶液製備金字塔結構 35
3.3 氮摻雜導電奈米鑽石之製備 36
3.3.1 以鑽石粉末及鈦金屬粉末震盪製備種子層 36
3.3.2 以微波電漿化學氣相沉積法成長奈米鑽石薄膜 37
3.4 濺鍍金屬修飾物 38
3.4.1 以射頻磁控濺鍍機濺鍍鎳金屬 38
3.4.2 以射頻磁控濺鍍機濺鍍氧化銅金屬氧化物 40
3.5 葡萄糖感測器試片封裝及循環伏安法表面改質 41
3.5.1 葡萄糖感測器試片封裝 41
3.5.2 葡萄糖感測器表面改質 42
3.6 實驗分析儀器介紹 42
3.6.1 場發射掃描式電子顯微鏡 ( FE-SEM ) 42
3.6.2 X射線繞射儀 (X-ray diffraction，XRD) 43
3.6.3 顯微拉曼光譜儀(Micro-Raman) 45
3.6.4 X射線光電子能譜儀 (X-Ray Photoelectron Spectroscopy，XPS) 46
3.6.5 原子力顯微鏡(Atomic Force Microscope，AFM) 47
3.6.6 傅利葉紅外線光譜儀(Fourier Transform Infrared spectrometer, FTIR) 48
3.6.7 電化學分析儀 (Electrochemical analyzer) 49
第四章　結果與討論 50
4.1 以不同結構成長摻雜氮的奈米鑽石薄膜之製備與特性比較分析 50
4.1.1 摻雜氮的奈米鑽石薄膜表面型態分析 50
4.1.2 摻雜氮的奈米鑽石薄膜拉曼光譜分析 52
4.1.3 摻雜氮的奈米鑽石薄膜X射線繞射儀分析 54
4.1.4 摻雜氮的奈米鑽石薄膜四點探針分析 55
4.1.5 摻雜氮的導電奈米鑽石葡萄糖靈敏度分析 56
4.2 不同厚度的氫氧化鎳/導電奈米鑽石薄膜特性比較分析 58
4.2.1 氫氧化鎳/導電奈米鑽石表面型態分析 58
4.2.2 摻雜氮的奈米鑽石薄膜拉曼光譜分析 66
4.2.3 氫氧化鎳/導電奈米鑽石X射線繞射儀分析 67
4.2.4 氫氧化鎳/導電奈米鑽石傅立葉紅外光譜分析 69
4.2.5 氫氧化鎳/導電奈米鑽石葡萄糖量測之電化學分析 70
4.2.5.a 循環伏安法分析 70
4.2.5.b 定電位沈積分析法分析(靈敏度分析) 74
4.2.5.c 定電位沈積分析法分析(選擇性分析) 82
4.2.5.d 定電位沈積分析法分析(穩定度分析-時間) 86
4.2.5.e 定電位沈積分析法分析(穩定度分析-溫度) 89
4.2.6 氫氧化鎳/導電奈米鑽石薄膜葡萄糖靈敏度分析 95
4.3 不同厚度的氧化銅/導電奈米鑽石薄膜特性比較分析 97
4.3.1 氧化銅/導電奈米鑽石表面型態分析 97
4.3.2 摻雜氮的奈米鑽石薄膜拉曼光譜分析 104
4.3.3 氧化銅/導電奈米鑽石X射線繞射儀分析 105
4.3.4 氧化銅/導電奈米鑽石傅立葉紅外光譜分析 106
4.3.5 氧化銅/導電奈米鑽石葡萄糖量測之電化學分析 107
4.3.5.a 循環伏安法分析 107
4.3.5.b 定電位沈積分析法分析(靈敏度分析) 110
4.3.5.c 定電位沈積分析法分析(選擇性分析) 118
4.3.5.d 定電位沈積分析法分析(穩定度分析-時間) 121
4.3.5.e 定電位沈積分析法分析(穩定度分析-溫度) 125
4.3.6 氧化銅/導電奈米鑽石薄膜葡萄糖靈敏度分析 131
4.4 各種薄膜材料葡萄糖靈敏度分析比較 133
第五章　結論與未來展望 137
5.1 結論 137
5.2 未來展望 140
參考文獻 141

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