開發石墨烯多孔碳電極搭配攜帶式裝置用於肌肝酸與白蛋白檢測

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黃俊諺(Huang,Chun,Yen) 查詢紙本館藏

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電機工程學系

論文名稱

開發石墨烯多孔碳電極搭配攜帶式裝置用於肌肝酸與白蛋白檢測

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摘要(中)

本研究採用網板印刷技術並將網印碳漿添加石墨烯(Graphene)與碳酸鈣(CaCO3)進行改良，開發出石墨烯多孔網印碳電極。透過循環伏安法(CV)研究電極對赤血鹽溶液之電化學性能，結果顯示石墨烯多孔碳電極比純碳電極電流響應高出2.4倍。電化學阻抗譜(EIS)量測實驗中，獲得石墨烯多孔碳電極與純碳電極之電荷轉移電阻分別為3.93 kΩ與7.02 kΩ，降低55%，並且透過電雙層電容值計算出表面積提升1.8倍。掃描式電子顯微鏡(SEM)下，觀察到電極表面孔洞與石墨烯層狀皺褶結構使得表面積提升，證實本研究開發出改良電化學特性之電極。
　　應用方面，以石墨烯多孔網印碳電極為基礎，製備出電流式肌酐酸(Creatinine)感測器與抗體式白蛋白(Albumin)感測器，用於檢測人體血液裡肌酐酸濃度與尿液裡白蛋白濃度，這兩者的濃度都是評估慢性腎臟病的重要指標。肌酐酸感測器是採用三酵素系統催化肌酐酸而增加氧化還原反應電流；純溶液實驗中，在濃度0500 μM區間能獲得具有高度決定係數(R2 = 0.994)之檢量線。並且在含有干擾物(尿酸、對乙醯氨基酚、抗壞血酸)的情況下，仍然獲得具有高度決定係數(R2 = 0.991)之檢量線，實驗結果誤差皆小於1.3%。白蛋白感測器則是利用抗原與抗體間的特異性吸附而降低電流響應；純溶液實驗中，在濃度10300 mg/L亦獲得了具有高度決定係數(R2 = 0.995)之檢量線。在含有干擾物(尿酸、葡萄糖、抗壞血酸、肌酐酸)的情況下，仍然能獲得具有高度決定係數(R2 = 0.994)之檢量線，實驗結果誤差小於2.8%。
　　此外，本研究改良攜帶式恆電位儀，整合肌酐酸與白蛋白兩種檢測平台，修改使用者選單，硬體方面則新增快閃記憶體(flash memory)與電源轉換器，使攜帶式恆電位儀能儲存一百筆量測記錄，並能用市面上常見3號(AA)乾電池驅動電路。攜帶式恆電位儀連接感測器後，可進行肌肝酸或白蛋白濃度檢測，實驗結果顯示，在含有干擾物情況下分別能獲得具有高度決定係數(R2 = 0.988，R2 = 0.992)之檢量線，其結果也和大型量測儀IM6ex量測結果誤差不到1.9%，人體樣品量測中平均誤差不到4%，與醫院檢測結果平均誤差約7%，證實該方便、簡易的裝置能用於肌酐酸與白蛋白之精準檢測。

摘要(英)

This study focused on the development of screen-printed graphene porous carbon electrode and portable potentiostat for detecting albumin and creatinine in clinical samples.
　　Screen-printed graphene porous carbon electrode was fabricated by mixing graphene and calcium carbonate (CaCO3) in carbon paste and printed on polycarbonate (PC) substrate. Cyclic voltammetry (CV) redox peak currents for graphene porous carbon electrode were 2.4 times higher than the bare carbon electrode. Electrochemical impedance spectroscopy (EIS) analysis showed that the charge transfer resistance of the graphene porous carbon electrodes and carbon electrode was 3.93 kΩ and 7.02 kΩ respectively, incorporation of graphene with carbon paste reduced the charge transfer resistance by 55%. From the electric double-layer capacitance value, it was inferred that the surface area of graphene porous carbon electrodes increased by 1.8 times. Scanning electron microscope (SEM) images revealed that the graphene porous carbon electrode surface exhibited porous structure with great number of holes and crumpled graphene nanosheets.
　　The developed screen-printed graphene porous carbon electrode sensor was employed for albumin detection in human urine and creatinine detection in human blood samples. With possible interferences, the sensor can detect albumin in the linear range from 10 to 300 mg/L with a coefficient of determination R2=0.994. In creatinine detection with interference, the calibration curve with a coefficient of determination R2=0.991 was obtained for the creatinine concentration range 0500 μM.
　　Portable potentiostat was developed with creatinine and albumin detection functions. Portable potentiostat consists of friendly user menu, flash memory to store hundred records and AA battery for power supply. The reformed portable potentiostat was used to detect creatinine or albumin by connecting creatinine sensor or albumin sensor. The calibration line with high coefficient of determination (R2=0.988, R2=0.992) was obtained for creatinine detection and albumin detection. The response of the potentiostat is similar to the commercial instrument IM6ex with error less than 1.9%. Confirmed that this portable potentiostat collocation graphene porous carbon electrodes can accurate and convenient detect albumin or creatinine. The graphene-based sensor and portable potentiostat proposed herein can be used for detecting albumin and creatinine accurately and user-friendly.

關鍵字(中)

★ 電化學
★ 肌酐酸
★ 白蛋白
★ 腎臟病
★ 網印碳電極

關鍵字(英)

★ Screen printed carbon electrode
★ kidney disease
★ albumin
★ creatinine
★ Electrochemistry

論文目次

摘要………………………………………………………………………………i
Abstract…………………………………………………………………..……. iv
致謝……………………………………………………………………..….……v
目錄………………………………………………………………………..……vi
圖目錄…………………………………………………………………..………xi
表目錄…………………………………………………………………...……xvii
第一章緒論 1
1-1腎臟病與肌酐酸和白蛋白的關係 1
1-1-1腎臟病 1
1-1-2肌酐酸 3
1-1-3人類血清白蛋白 4
1-2電化學簡介 5
1-2-1電化學量測法 5
1-2-2電化學感測器 10
1-3石墨烯簡介 11
1-3-1石墨烯 11
1-3-2石墨烯的應用 12
1-4恆電位儀 13
1-4-1恆電位儀原理 13
1-4-2攜帶式恆電位儀 14
1-5文獻回顧 15
1-5-1石墨稀特性與應用 15
1-5-2肌酐酸感測器 18
1-5-3白蛋白感測器 21
第二章研究動機與目的 26
2-1 研究動機 26
2-2研究目的 27
第三章實驗方法 28
3-1攜帶式恆電位儀製作 28
3-1-1攜帶式恆電位儀架構 28
3-1-2硬體 29
3-1-3程式撰寫 35
3-1-4數據輸出 36
3-2改良攜帶式恆電位儀 37
3-2-1加裝記憶體 37
3-2-2加裝電源轉換器 40
3-2-3使用者介面修改 41
3-3開發石墨烯多孔網印碳電極 43
3-3-1材料與儀器 43
3-3-2印製電極 47
3-3-3石墨烯含量最佳化實驗 49
3-3-4掃描式電子顯微鏡 49
3-3-5電子轉移速率常數 50
3-3-6電化學阻抗譜 52
3-4肌肝酸量測實驗 53
3-4-1材料與儀器 53
3-4-2肌酐酸感測器製作 56
3-4-3純溶液檢測 56
3-4-4干擾物實驗 57
3-4-5人體血液樣品量測 59
3-5白蛋白量測實驗 59
3-5-1材料與儀器 59
3-5-2白蛋白感測器製作 62
3-5-3純溶液檢測 63
3-5-4干擾物實驗 64
3-5-5人體尿液樣品量測 66
第四章實驗結果 67
4-1攜帶式恆電位儀的實現 67
4-1-1電路實體 67
4-1-2操作介面 69
4-1-3實際量測 71
4-2石墨烯多孔網印碳電極特性分析 73
4-2-1石墨烯含量最佳化 73
4-2-2掃描式電子顯微鏡 79
4-2-3電子轉移速率常數 80
4-2-4電化學阻抗譜 84
4-3肌酐酸量測實驗結果 88
4-3-1純溶液檢測 88
4-3-2干擾物實驗 92
4-3-3人體血液樣品量測 101
4-4白蛋白量測實驗結果 106
4-4-1純溶液檢測 106
4-4-2干擾物實驗 110
4-4-3人體尿液樣品量測 121
第五章結論 126
第六章未來展望 128
參考文獻 ……………………………………………………………………...125

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指導教授

蔡章仁(Jang-Zern Tsai)

審核日期

2016-8-29

推文