Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/3662
標題: 多層壁奈米碳管-三氧化二鋁包覆二氧化矽奈米顆粒複合材料薄膜作為生物感測器之探討
Biosensors based on multiwalled carbon nanotubes - alumina-coated silica nanoparticles composite films
作者: 蔡明潔
Tsai, Ming-Chieh
關鍵字: carbon nanotube;奈米碳管;alumina-coated silica nanoparticles;glucose oxidase;glucose biosensor;三氧化二鋁包覆二氧化矽奈米顆粒;葡萄糖氧化酵素;葡萄糖生物感測器
出版社: 化學工程學系所
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摘要: 
本論文第一部份以一種新穎的非共價鍵與非有機溶液修飾的方式藉由奈米顆粒來分散奈米碳管於水溶液中,多層壁奈米碳管(multi-walled carbon nanotubes, MWNTs)被帶有高正電荷之三氧化二鋁包覆二氧化矽奈米顆粒(alumina-coated silica nanoparticles, ACS)直接分散於水溶液中,而沒有將MWNTs的表面官能基化。經由穿透式電子顯微鏡及原子力顯微鏡的微觀表面形貌分析,可以確定帶正電荷之ACS奈米顆粒確實可圍繞於MWNTs之上,且可有效的將MWNTs彼此間分散開來。探討水溶液的pH值、ACS奈米顆粒於水溶液中的量、以及MWNTs於水溶液中的量,對於MWNTs的分散有何影響,而去設計一連串的實驗,在經過超音波震盪一小時後,觀察MWNTs的分散情形。接著,我們將MWNTs-ACS複合材料以自組裝的方式吸附於玻璃碳電極(glassy carbon electrode, GCE)表面,以原子力顯微鏡觀察MWNTs-ACS複合材料吸附在GCE表面之情形,發現MWNTs在GCE表面扮演奈米導線的角色,提供良好的電傳導性。MWNTs-ACS複合材料薄膜修飾GCE浸於含有5 mM Fe(CN)63-/4-氧化還原物的0.1 M氯化鉀(potassium chloride, KCl)溶液系統中,分別以不同的掃描速度(25~200 mV/s)掃描之循環伏安實驗中,我們可以觀察到隨著掃描速度不斷的增加,除了會使得陽極的峰電流及陰極的峰電流增加,而且陽極峰電流及陰極峰電流分別與掃描速率的平方根成正比的線性關係,因此可以判斷出由MWNTs-ACS複合材料薄膜修飾GCE所進行的電化學反應屬於擴散控制。我們將MWNTs-ACS複合材料薄膜修飾GCE做為化學感測器偵測過氧化氫(hydrogen peroxide, H2O2)與還原型煙胺腺嘌呤二核酸(β-nicotinamide adenine dinucleotide, reduced form, NADH)時,發現可用較小之電壓即可催化H2O2與NADH,而得到相當高之電流訊號。
本論文第二部份先以電化學沉積將鉑(platimum, Pt)奈米顆粒導入MWNTs-ACS複合材料薄膜中,再將葡萄糖氧化酵素以離子結合法藉由靜電吸附固定在MWNTs-ACS-Pt複合材料薄膜中,其表面形貌、元素成分與效能測定分別利用場發射掃描式電子顯微鏡、X光能量散譜儀、循環安伏法與安培法進行測試。其最佳化葡萄糖生物感測器之線性範圍可達10.5 mM,其靈敏度高達113.13 mA M -1cm-2,偵測極限為6.18 μM,應答時間約5 sec。最後為了加強其穩定度與對干擾物的測定,我們在該葡萄糖生物感測器的電極表面,再加上一層全氟磺酸聚合物作為保護。

A novel noncovalent and inorganic method was used to disperse multi-walled carbon nanotubes (MWNTs) in aqueous solution. MWNTs were directly dispersed into highly charged alumina-coated silica nanoparticles (ACS) aqueous solution without functionalization of their surfaces. The dispersed MWNTs was characterized by transmission electron microscopy and atomic force microscopy. It was possible to disperse up to 20 mg/mL of MWNTs in 1 wt% ACS nanoparticles aqueous solution at pH 2. This homogeneous MWNTs-ACS aqueous solution was stable for weeks after ultrasonication.
A novel method for attaching MWNTs-ACS composite onto the surface of glassy carbon electrode (GCE) by a self-assembly process is described. The resulting MWCNT-ACS modified GCE was investigated by atomic force microscopy. In cyclic voltammetric responses, both anodic and cathodic peak currents varied linearly with the square root of scan rates in 0.1 M KCl containing 5 mM Fe(CN)64- at MWNTs-ACS modified GCE, which suggests a diffusion-controlled process. The MWNTs-ACS modified GCE exhibits the abilities to raise the current responses and to decrease the electrooxidation potential of β-nicotinamide adenine dinucleotide, reduced form (NADH) and hydrogen peroxide (H2O2).
A novel amperometric glucose biosensor based on electrodeposition of Pt nanoparticles on MWNTs by potentiostatic method and electrostatic adsorption of glucose oxidase (GOD) at the MWNTs-ACS-Pt-GOD modified GCE is described. The morphology, nature, and performance of the MWNTs-ACS-Pt-GOD nanobiocomposite were characterized by field emission scanning electron microscopy, energy dispersive X-ray spectroscopy, cyclic voltammetry, and amperometry. The glucose biosensor displayed a linear range up to 10.5 mM, a sensitivity of 113.13 mA M -1cm-2, a detection limit of 6.18 μM, and a response time of less than 5 s. Finally, to improve the stability and anti-interferent ability of the glucose biosensor, Nafion film was coated on the surface of the MWNTs-ACS-Pt-GOD modified GCE.
URI: http://hdl.handle.net/11455/3662
其他識別: U0005-0207200809574500
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