以導電性聚苯胺建構過氧化氫生物感測器之技術及其性質探討

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題名:	以導電性聚苯胺建構過氧化氫生物感測器之技術及其性質探討
其他題名:	The techniques and characterizations for constructing hydrogen peroxide biosensors by conductive polyaniline
作者:	陳建中 Chen, Chien-Chung
貢獻者:	杜景順;顧野松 Do, Jing-Shan;Gu, Ye-Song 東海大學化學工程與材料工程學系
關鍵詞:	過氧化氫;生物感測器;辣根過氧化酵素;聚苯胺 hydrogen peroxide;biosensor;horseradish peroxidase;polyaniline;SBA-15
日期:	2009
上傳時間:	2011-02-22T07:44:28Z (UTC)
摘要:	本論文中以導電性聚苯胺(PANI)為電極表面修飾高分子，以循環伏安法(CV)聚合PANI於Pt/Al2O3電極表面製備成PANI/Pt/Al2O3電極，再使用電吸附法固定化HRP酵素並以戊二醛(GA)為交聯劑，製備GA-HRP/PANI/Pt/Al2O3電極。另外，在PANI聚合過程中添加牛血清蛋白(BSA)，分別製備為PANI(BSA)/Al2O3與GA-HRP/PANI(BSA)/Al2O3兩種電極。此外，研究過程中亦合成中孔矽材料SBA-15，作為HRP固定化的載體，應用於GA/SBA-15(HRP)/PANI/Pt/Al2O3電極的製備。將上述製備所得的電極使用CV法感測過氧化氫，探討電極之感測特性。另外，探討了溶氧對於PANI/Pt/Al2O3電極感測過氧化氫的影響，並嘗試添加除氧劑於感測系統中，去除溶氧的影響。分別以GA-HRP/PANI/Pt/Al2O3與GA-HRP/PANI(BSA)/Pt/Al2O3電極於0.1 M磷酸鹽緩衝溶液(pH 6.2)中感測過氧化氫，其感測濃度線性範圍為10 μM ~ 23.9 mM與10 μM ~ 35.2 mM，感測靈敏度由37.55提升至44.31 μA mM-1。在穩定性測試，分別使用PANI/Pt/Al2O3與PANI(BSA)/Pt/Al2O3電極於17天中21次感測2.39 mM的過氧化氫，可發現在第17天的剩餘感測活性由PANI/Pt/Al2O3電極的40.8 %提升至PANI(BSA)/Pt/Al2O3電極的80.5 %，顯示PANI中包埋BSA對於感測的靈敏度與穩定性有顯著的提升。在干擾測試方面，分別添加濃度為0.5 mM的尿酸、尿素與維它命C於含有2.39 mM過氧化氫的感測系統中，對於GA-HRP/PANI/Pt/Al2O3電極的感測靈敏度與還原電流的影響皆小10 %。在GA-HRP/PANI/Pt/Al2O3與GA/SBA-15(HRP)/PANI/Pt/Al2O3電極比較部份，於0.1 M磷酸鹽緩衝溶液(pH 6.2)中感測過氧化氫，感測濃度線性範圍皆為10 μM ~ 23.9 mM，GA/SBA-15(HRP)/PANI/Pt/Al2O3電極的靈敏度由不含SBA-15的37.55 μA mM-1下降至25.05 μA mM-1，於16天中15次感測1.96 mM的過氧化氫，在第16天的感測剩餘感測活性由GA-HRP/PANI/Pt/Al2O3電極的40.5 %提升至PANI(BSA)/Pt/Al2O3電極的75.2 %，顯示HRP酵素固定於SBA-15中對於活性的穩定有明顯的幫助。使用除氧劑去除溶液中溶氧的影響部份，實驗結果顯示添加硫代硫酸鈉可有效去除溶液中溶氧，當添加濃度小於1 mM時，可有效去除溶液中的溶氧並不會影響過氧化氫的感測濃度。 In this study, the PANI or PANI(BSA) films was electrochemically synthesized on the Pt/Al2O3 base to form the PANI/Pt/Al2O3 or PANI(BSA)/Pt/Al2O3 electrode, and horseradish peroxidase (HRP) was then immobilized in PANI or PANI(BSA) films to construct the GA-HRP/PANI/Pt/Al2O3 or GA-HRP/PANI(BSA)/Pt/Al2O3 biosensor. Furthermore, the mesoporous silica SBA-15 was prepared and was employed to entrap HRP in order to construct a GA/SBA-15(HRP)/PANI/Pt/Al2O3 electrode. The properties and the performances of those bio-electrodes were fully investigated. Moreover, the influence of the dissolved oxygen on sensing of hydrogen peroxide with those PANI modified electrode was discussed and the possible elimination was proposed by using oxygen scavengers.For electrodes, such as GA-HRP/PANI/Pt/Al2O3 and GA-HRP/PANI(BSA)/Pt/Al2O3, the linear correlation for sensing hydrogen peroxide in a 0.1 M phosphate buffer were obtained in the range of 10 μM ~ 23.9 mM and 10 μM ~ 35.2 mM, respectively, while the sensitivities were 37.55 and 44.31μA mM-1, respectively. By comparing the stability after sensing 2.39 mM hydrogen peroxide for twenty-one times in a 17-day period, the percentage of residual response current were 40.8 % for PANI/Pt/Al2O3 and 80.5 % for PANI(BSA)/Pt/Al2O3, indicating that BSA was useful for improving the sensitivity and stability of PANI modified hydrogen peroxide biosensor. In addition, 0.5 mM of uric acid, urea, or ascorbic acid would cause less than 10% reduction of cyclic voltammetry (CV) current on sensing 2.39 mM hydrogen peroxide for GA-HRP/PANI/Pt/Al2O3. For the electrode GA/SBA-15(HRP)/PANI/Pt/Al2O3, the linear correlation and the sensitivity for sensing hydrogen peroxide sensor in a 0.1 M phosphate buffer were obtained in the range of 10 ~ 23.9 mM and 25.05 μA mM-1, respectively. After sensing 1.96 mM hydrogen peroxide for fifteen times in a 16-day period, the percentage of residual response current were 75.2 %, which was better than that of GA-HRP/PANI/Pt/Al2O3 (40.5%), implicating that SBA-15 was also able to stabilize the entrapped HRP and therefore improved the performance of the constructed biosensor. Finally, we demonstrated the influence of the dissolved oxygen on sensing hydrogen peroxide with PANI modified electrodes, and we proposed strategies to eliminate the influences. Our results inindicated that the oxygen scavenger such as sodium thiosulfate was able to effectively remove the dissolved oxygen, thereby reduce its effect on the performance of electrode, Meanwhile, sodium thiosulfate displayed the negligible effect on hydrogen peroxide measurements while its applied concentration was below 1 mM.
顯示於類別:	[化學工程與材料工程學系所] 碩博士論文

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