利用碳奈米材料製備酵素型生物感測器及電分析應用

Fabrication of enzymatic biosensors using carbon nanomaterials for electroanalytical applications

Ezhivilian.A.T(Ezhivilian.A.T)

指導教授 ： 陳生明

國立臺北科技大學/工程學院/能源與光電材料外籍生專班研究所/博士(2014年)

https://doi.org/10.6841/NTUT.2014.00885

摘要

本研究主要集中在製備第三代酵素型生物感測器基於碳奈米材料偵測各種生物學上重要的化合物，例如過氧化氫、葡萄糖和有害的無機化合物，如碘酸亞硝酸鹽和溴酸鹽。使用供固定酵素的奈米材料包括碳奈米管、還原石磨烯氧化物、金屬與金屬氧化物奈米材料。利用各種方法製備酵素型生物感測器已被用於各種電催化應用中。第一章介紹一種新穎的複合膜通過簡單的化學還原步驟包括官能基化多層奈米碳管、L-lysine和氧化鋅奈米複合材料的製備方法。所製備的複合物，用作為固定化基質的血紅蛋白，製備一個過氧化氫和溴酸的生物感測器。所提出的生物感測器提供了一個寬的線性範圍，小的Michealis-Menten常數與良好的穩定性和重複性。第二章論述了製備第三代生物感測器，利用過氧化氫酵素固定到L-lysine與多層奈米碳管複合膜來偵測過氧化氫與IO3-.所提出的L-lysine/ multiwalled複合膜提供了過氧化氫酶適宜的微環境，這有助於增強對直接電化學和保持其生物活性。此生物感測器有易於製造、選擇性好，偵測線性範圍寬的優點。第三章的重點含功能化的multi-walled carbon nanotubes-Tyramine-Au，透明的奈米複合膜，通過對肌紅蛋白固定在玻璃碳電極表面的共價交聯的方式製備。所提出的生物感測器具有可還原過氧化氫與氧化亞硝酸鹽的優異電催化活性，可應用於生物感測器與易於簡單操作的環境條件下進行。第四章重點製備的二氧化錳和化學還原的石墨烯氧化物膜為Glucose Oxidase/poly-L-lysine的固定化。該生物感測器的製造是簡單方便，不需要有毒的試劑和不涉及任何複雜的多步驟過程。所提出的生物感測器具有低的成本，可得知再現性，重複性，長期穩定性與靈敏的優點是有前途的用於葡萄糖存在於臨床和環境分析食物的測定。

關鍵字

奈米碳管 ； 化學還原石磨烯氧化物 ； 胺基酸 ； 電分析 ； 過氧化氫

並列摘要

This thesis mainly focuses on the fabrication and characterization of third-generation enzymatic biosensors based on carbon nanomaterials for the determination of various biologically important compounds such as hydrogen peroxide, and glucose, and toxic inorganic compounds such as iodate nitrite and bromate. The nanomaterials used for the immobilization of enzymes include carbon nanotubes, chemically reduced graphene oxide, metal and metal oxide nanomaterials. The enzymatic biosensors constructed using various approaches have been used for various electrocatalytic applications. The Second chapter describes the preparation of a novel composite film consisting of functionalized multi-walled carbon nanotubes, L-histidine and ZnO nanocomposite via a simple chemical reduction procedure. The as-prepared composite was then used as the immobilization matrix for hemoglobin to construct a mediator-free H2O2 and bromate biosensor. The proposed biosensor provides a wide linear range, small Michealis-Menten constant, favorable stability and reproducibility. Third chapter deals with the construction of a novel third-generation biosensor based on the immobilization of catalase onto L-lysine and multiwalled carbon nanotube film for the determination of H2O2 and IO3-. The proposed L-lysine/multiwalled carbon nanotube composite film provided a suitable microenvironment for catalase, which helps for enhanced direct electrochemistry and maintaining its bioactivity. This biosensor has the advantages of ease of fabrication, good selectivity and wide linear range of detection. Fourth chapter focuses on the construction of a flexible, transparent nano composite film containing functionalized multi-walled carbon nanotubes-tyramine-Au through a covalent cross-linking approach on a GCE electrode surface for the immobilization of myoglobin. The proposed biosensor exhibited excellent electrocatalytic activity towards the reduction of H2O2 and oxidation of nitrite with the advantages of simple approaches used for the construction of biosensor and easy to operate under ambient conditions. Fifth chapter focus on the preparation of MnO2 and chemically reduced graphene oxide film for the immobilization of Glucose Oxidase/poly-L-lysine. The biosensor fabrication is simple and convenient, not requiring toxic reagents and not involving any complex multistep process. The proposed biosensor with the advantages of low-costs, appreciable reproducibility, repeatability, long term stability and sensitive sensing approach is promising for the determination of glucose present in the clinical and environmental food analysis.

並列關鍵字

Carbon nanotubes ； Chemically reduced graphene oxide ； Amino acid ； Electro catalysis ； Hydrogen peroxide

參考文獻

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