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研究生： 林書宇
Lin, Shu-Yu
論文名稱： ABTS複合奈米碳管修飾電極應用於伏安法檢測尿液白蛋白之研究
A study on the application of ABTS/carbon nanotube modified electrode for the voltammetric detection of urine albumin
指導教授： 林家裕
Lin, Chia-Yu
學位類別： 碩士
Master
系所名稱： 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年： 2021
畢業學年度： 109
語文別： 中文
論文頁數： 106
中文關鍵詞： 人血清白蛋白 、2, 2’-聯氮-雙(3-乙基-苯并噻唑啉-6-磺酸) 、奈米碳管 、降解產物 、伏安法感測器 、尿液
外文關鍵詞： Human serum albumin, ABTS, Carbon nanotube, Degradation products, Voltammetric sensor, Urine
相關次數： 點閱：145  下載：0 
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    • 尿液中白蛋白的濃度是評估身體健康狀況的重要指標，若能夠在慢性腎臟病的初期就透過微白蛋白尿及早發現腎功能異常並進行就醫治療，患者便可藉由藥物、飲食、運動等恢復到健康狀態。現有白蛋白定量檢測技術主要採用免疫化學方式，多使用高成本與需低溫保存之生物試劑(如酵素、生物抗體等)，且需大型檢測儀器與專業人員操作，故不適合例行篩檢與居家照護，因此開發簡易、高準確性且可直接應用於檢測尿液中白蛋白的感測器對於臨床與預防醫學領域是重要的。
    本研究利用經循環伏安法前處理後之2, 2’-聯氮-雙(3-乙基-苯并噻唑啉-6-磺酸)與奈米碳管與修飾電極(CNT-ABTS)，吸附並電催化氧化白蛋白，並以其電流訊號作為白蛋白濃度檢測之依據。且當電極經循環伏安法前處理後，電極上ABTS的降解產物可利用氫鍵吸附更多白蛋白分子中的酪胺酸和色胺酸，因此靈敏度提升至原本的3.5倍。干擾物測試發現尿酸的吸附與干擾最為明顯，因此我們針對尿酸與白蛋白於CNT-ABTS修飾電極上之吸附行為與作用力進行探討，結果顯示兩者皆為不可逆反應和吸附控制，並經吸附曲線之動力學和熱力學分析，發現白蛋白較偏向二級動力吸附，且其與電極之作用力為尿酸的約10.9倍。最後，所開發之電化學感測器對白蛋白具有高選擇性辨識與催化功能，檢測時不須額外加入試劑並具有優良感測性能，包括高靈敏度(0.0040mA cm-2 ppm-1)、低偵測下限(4 ppm)、寬線性範圍(10-100 ppm)、低應答時間(30分鐘)、高保存穩定性(28天)、高重複使用次數(5次)，以及於尿液實測中具高準確性(誤差<15%)。

    The concentration of urine albumin is significant indicator for assessing human health. If chronic kidney can be early detected during microalbuminuria, people can restore through regular medication, diet and exercise. Nowadays, the sensing methodologies for HSA mainly adopt immunochemical methods, which require high-cost reagents, large-scale instruments and professional operation, preventing them from the practical application in routine screening and home care. Consequently, the development of simple and low-cost sensing platform that can be directly applied for the detection of urine albumin is highly urgent and essential for clinical and preventive medicine.
    In this study, (2,2’-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid))/multi-walled carbon nanotube nanocomposite (ABTS/CNT) modified electrode was fabricated and its application for the voltammetric detection of urine albumin was investigated. It was found that cyclic voltammetry (CV) pretreatment of the ABTS/CNT modified electrode enriches the number of active sites to the oxidation of tyrosine and tryptophan residues of albumin, resulting in significant enhancement in the electrocatalytic activity (~3.5 times) compared with as-prepared one. From the interference test, we found that uric acid is the mostly interference substance. Therefore, we investigated the adsorption behaviors and interactions of uric acid and HSA adsorbed onto the electrode, and the results showed that both are irreversible reaction (two electrons transfer) and adsorption-limited. We further analyzed the kinetics and thermodynamics of the adsorption curves and found that the adsorption of HSA onto electrode follows pseudo-second order sorption kinetics, and the interaction between HSA and SPCE/CNT-ABTSCV electrode is 10.9 times higher than that of uric acid. Under the optimized conditions, the CV-pretreated ABTS/CNT modified electrode exhibited promising sensing characteristics towards the detection of urine albumin, including high sensitivity (0.004 mA cm-2 ppm-1), low limit of detection (4 ppm) (S/N = 3), wide linear range (10-100 ppm), low response time (30 min), long-term stability (28 days), good reusability (5 cycles), and high accuracy of urine detection (within 15% deviation).

    摘要 I Extended Abstract II 致謝 XIII 總目錄 XIV 表目錄 XVI 圖目錄 XVIII 第一章 緒論 1 1.1 前言 1 1.2 感測器 2 1.2.1 基本結構與工作原理 2 1.2.2 辨識單元 4 1.2.3 辨識單元於傳感器之修飾 5 1.2.4 傳感器 7 1.3 白蛋白 9 1.3.1 白蛋白介紹 9 1.3.2 白蛋白感測器的開發 11 1.4 研究動機 14 第二章 原理與文獻回顧 16 2.1 奈米碳管的特性 16 2.2 ABTS的電化學特性 17 2.3 電化學原理 22 2.3.1 化學反應程序 22 2.3.2 循環伏安法 23 2.4 吸附動力學 25 第三章 實驗方法 27 3.1 實驗藥品 27 3.2 實驗儀器 28 3.3 溶液配製 28 3.4 電極製備 29 3.5 感測電極電化學分析 29 3.5.1 電化學系統 29 3.5.2 電化學步驟及參數 30 3.6 實際尿液應用 30 3.7 物性分析方法 31 3.7.1 拉曼光譜儀 31 3.7.2 X-ray光電子能譜儀 32 第四章 結果與討論 33 4.1 電極物性分析 33 4.1.1 拉曼光譜 33 4.1.2 X-ray光電子能譜 36 4.2 感測效能分析 40 4.2.1 不同修飾電極之影響 40 4.2.2 有無前處理之影響 45 4.2.3 干擾物之影響 52 4.2.4 緩衝溶液的浸泡與感測pH值之影響 57 4.2.5 電極漿料中ABTS濃度之影響 59 4.2.6 實際尿液分析 64 4.2.7 電極可重複感測次數測試 65 4.2.8 電極穩定性測試 66 4.3 感測機制 70 4.3.1 電極前處理之電化學行為 70 4.3.2 尿酸與白蛋白於電極上之電化學行為 72 4.3.3 尿酸與白蛋白之電子轉移數 75 4.3.4 尿酸與白蛋白之吸附曲線 76 4.3.4.1 吸附曲線之動力學 77 4.3.4.2 吸附曲線之熱力學 90 第五章 結論與未來展望 92 5.1 結論 92 5.2 建議與展望未來 93 第六章 參考文獻 94 附錄 99

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