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標題: | 奈米結構修飾電極應用於催化型生物感測器與親和性適體感測器 Nanostructural Modified Electrode for Catalytic-based Biosensors and Affinity-based Aptasensors |
作者: | Min-Han Lee 李旻翰 |
指導教授: | 何國川(Kuo-Chuan Ho) |
關鍵字: | 適體感測,碳材,電化學修飾電極,電化學感測器,官能化奈米粒子,自組裝薄膜沉積,普魯士藍, Aptasensor,Carbon material,Chemically modified electrode,Electrochemical sensor,Functional nanoparticles,Nano-assembled deposition,Prussian blue, |
出版年 : | 2018 |
學位: | 碩士 |
摘要: | 本論文主要關注化學修飾電極於電化學生物感測之應用。可將本論文分成兩大部分,分別針對催化型感測器和親合型感測器之製備與其機制進行深入與系統性的探討。第三章主要討論催化型感測器,利用白金奈米粒子修飾之石墨烯奈米緞帶結構用於過氧化氫和烟酰胺腺嘌呤二核苷酸 (NADH)之生物感測。第四章則著重於親合型感測器,利用官能化之奈米普魯士藍粒子做為凝血酶適體生物感測器。
本論文的第一部分,我們成功的利用極少量的硫酸(10 ml/mg , 和文獻比較約減量90%),拆解石墨烯合成了石墨烯奈米緞帶結構。為了提升其電化學分析之性能,白金奈米粒子被修飾到奈米緞帶結構之表面以增加其導電度和催化性。從材料分析和電化學性質之測量,我們可以發現白金修飾後的複合材料有較低的電子傳導阻力並且可視為連結奈米緞帶結構之導電樞紐。做為一個催化型的生物感測器,此複合材料成功的降低了反應之電位並提升其感測之靈敏度。我們成功的利用白金奈米粒子和石墨烯奈米緞帶結構之複合材料製備了高靈敏度(378.5 (H2O2) 和 724.3(NADH) μA mM–1 cm–2)、高選擇性且穩定之電化學感測器。 本論文的第二部分,我們開發了新的成膜技術來沉積普魯士藍電化學薄膜。羧基修飾的普魯士藍奈米粒子可透過氫鍵自組裝到氧化銦錫玻璃上(利用控制組實驗和表面化學分析推導而知)。此成膜方法之膜厚可由沉積時間來控制,在控制的環境下約可以每四小時一層的速率沉積成普魯士藍修飾之薄膜。我們選擇凝血酶來證明此系統可以發展為親和性感測之平台。實驗之結果顯示,此修飾電極對於凝血酶有很廣之感測範圍 (1 pM-100 nM)與極低之交叉反應性(高選擇性)。更值得一提的是,此感測器具有可重複使用的特性,經過10次的再生後仍然有將近100%的電流訊號表現。這些結果顯示此系統除了可以設計於適體型之感測,更可以延伸到其他生物分子交互作用的應用。 This thesis aimed to develop chemically modified electrode for the application of biosensor. This thesis could be divided into two major parts including platinum nanoparticle decorated graphene nanoribbon (PtNPs/RGONRs) for NADH and H2O2 sensing (Chapter 3); and functionalized Prussian blue particles (fPBNPs) for thrombin aptasensing (Chapter 4). For the first part, we successfully synthesized graphene nanoribbons from unzipping carbon nanotubes with little amount of H2SO4 usage (10 ml/mg, 90% reduced comparing to literature). To enhance the analytical performance, we incorporate platinum nanoparticle to evaluate the conductivity and catalytic ability. Material characterizations and electrochemical measurement indicated that PtNPs could reduce the charge transfer resistance and played as a conductive node to synergize the nanoribbon structure. The composite material could successfully lower the formal potential of the reaction and improve the sensitivity. We achieve high sensitivity (378.5 (H2O2) and 724.3(NADH) μA mM–1 cm–2), great selectivity toward interferences and acceptable stability for practical use with the PtNPs/GNR modified electrode. For the second part, we developed a new method to deposit Prussian blue electroactive thin film. The carboxyl functional group anchoring on PB crystal could self-assemble onto ITO surface via hydrogen bonding (The mechanism was deduced from control experiment and surface property characterization). The film thickness could be controlled by time of deposition with a growth rate of one layer per four hours. Thrombin was chosen as the target to proof the concept of building an affinity-based aptasensor. We achieved a wide range of dynamic range (1 pM – 100 nM) and low cross-reactivity with non-target proteins. Moreover, the PB aptasensor was reusable and retained nearly 100% signal response after 10 cycles of repeated thrombin sensing. As can be expected, the present fPBNP sensing system can be extended to biomolecular interaction assay applications in addition to aptasensing. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/77612 |
DOI: | 10.6342/NTU201801877 |
全文授權: | 未授權 |
顯示於系所單位: | 化學工程學系 |
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