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標題: Glucose Biosensors Based on Multiwalled Carbon Nanotubes/Nafion/GOD Nanocomposite and Multiwalled Carbon Nanotubes/Polypyrrole/GOD Nanocomposite
作者: 黎世棊
Li, Shih-Ci
關鍵字: Multiwalled Carbon Nanotubes
出版社: 化學工程學系
摘要: Novel electroanalytical sensing nanobiocomposite materials are reported. Two methods of preparation of the glucose biosensors based on multi-walled carbon nanotubes (MWNTs) are investigated. The first one is prepared by a simple cast deposition on glassy carbon electrodes (GCE) with mixing MWNTs, Nafion, and a glucose oxidase (GOD) in appropriate amounts. The MWNTs are cylindrical with a diameter in the range of 40 - 60 nm and with a length of up to several micrometers and provide electrical conductivity. Nafion acts as a polymer backbone to give stable and homogeneous cast thin films. The resulting biosensing composite material is inexpensive, reliable, and easy to use. The homogeneity of the MWNTs/Nafion/GOD nanobiocomposite films was characterised by atomic force microscopy (AFM). Amperometric transducers fabricated with these materials were characterized electrochemically using amperometry in the presence of hydrogen peroxide and in the presence of glucose. Their linear response to hydrogen peroxide was demonstrated. This glucose biosensor sensitivity was strongly influenced by glucose oxidase concentration within the nanobiocomposite film. The optimized glucose biosensor (2.5 mg/ml GOD) displayed a sensitivity of 330 nA/mM, a linear range up to 2 mM, a detection limit of 4 μM, and a response time of less than 3 s. The another one is prepared by electrochemical technique. A nanobiocomposite film of polypyrrole (PPy), the functionalization of multi-walled carbon nanotubes (cMWNTs) and GOD were synthesized by electropolymerization which the PPy, MWNTs and GOD were deposited on the GCE simultaneously. The morphology of PPy/cMWNTs nanocomposite film was characterized by AFM and scanning electron microscope (SEM). The amounts of hydrogen peroxide and the heights of amperometric response of PPy/cMWNTs nanocomposite film vary proportionately. The results indicate that the electroanalytical PPy/cMWNTs/GOD nanobiocomposite film was highly sensitive and suitable for glucose biosensors. Relevant parameters of the film preparation were examined and optimized. The optimized glucose biosensor (1.5 mg/ml GOD) displayed a sensitivity of 95 nA/mM, a linear range up to 4 mM, a detection limit of 106 μM, and a response time of less than 8 s.
本研究成功的研究出奈米生物薄膜(nanobiocomposite)用於葡萄糖生物感測器,並且以兩種固定奈米碳管(multiwall carbon nanotubes, MWNTs)的方法做探討。首先利用簡單的方法將適當比例之奈米碳管、全氟磺聚合物(Nafion)及葡萄糖酵素(glucose oxidase, GOD)複合材料修飾玻璃碳電極。其中MWNTs的直徑為40-60 nm,長度為數微米長。以Nafion為此薄膜的脊柱使其穩定且呈現均勻。MWNTs/Nafion/GOD複合材料表面形態經由原子力顯微鏡觀察後,得知奈米碳管均勻的分布於Nafion之中。由電化學之安培法對過氧化氫測試,MWNTs/Nafion修飾電極與未修飾相較之下具有相當大的電流信號,且過氧化氫的濃度與電流成線性比例。將不同的葡萄糖酵素量加入MWNTs/Nafion中所製作成的葡萄糖生物感測器,其對於葡萄糖的偵測信號有相當大的影響。葡萄糖生物感測器GOD最適值為2.5 mg/mL,其靈敏度330 nA/mM、線性範圍達2 mM、偵測極限4 μM及應答時間3秒。 另外一種製作葡萄生物感測器方法為利用電化學的方式。以聚吡咯(polypyrrole, PPy)、官能基化的奈米碳管(cMWNTs)及GOD以電化學聚合同時將其沉積於玻璃碳電極上。PPy/cMWNTs薄膜以AFM及SEM觀察其表面形貌。PPy/cMWNTs的奈米複合薄膜對於過氧化氫具有高的訊號及呈線性比例。PPy/cMWNTs/GOD具有高的靈敏度非常適合用於葡萄感測器,試驗且找出關於膜的製備參數,其葡萄糖生物感測器GOD最適值為1.5 mg/mL GOD,其靈敏度95 nA/mM、線性範圍達4 mM及偵測極限106 μM及應答時間為8秒。
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