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標題: 石墨烯奈米薄膜作為電化學感測器及生物感測器之探討
Electrochemical sensor and biosensor based on graphene nanocomposite
作者: 林恩如
Lin, En-Ru
關鍵字: 聚吡咯;Graphene;全氟磺酸聚合物;電化學感測器;Nafion;polypyrrole;electrochemical sensors
出版社: 化學工程學系所
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本研究成功的利用簡單且快速的方法來製備以石墨烯(rGO)為主要材料之感測器。本論文分成三部份,第一部分主要探討以改良後的Hummers method製備出氧化石墨烯(GO),利用電子顯微鏡及原子力顯微鏡觀察其表面形貌。再以抗壞血酸將GO還原成rGO,以UV-Vis光譜儀及電化學方式觀察其還原的狀況,證實此方法卻實製備出氧化石墨烯(GO)及還原成石墨烯(rGO)。

第二部份以非共價鍵修飾方式藉由Nafion高分子來分散rGO並修飾於玻璃碳電極(GCE)上作為乙醯胺酚及阿斯匹靈感測器之應用。以電子顯微鏡觀察rGO/Nafion 修飾電極的表面形貌,得知rGO均勻的分散於電極表面上,接著利用循環伏安法及方波伏安法來研究所製備的rGO/Nafion/GCE對於乙醯胺酚及阿斯匹靈之電化學特性。相較於未修飾的GCE發現rGO/Nafion/GCE在偵測乙醯胺酚及阿斯匹靈下均具有較好的電流信號,顯示rGO具有良好的電催化效果。此外rGO/Nafion/GCE對於乙醯胺酚及阿斯匹靈的效能參數分別是靈敏度50.77 AM-1cm-2和3.521AM-1cm-2,偵測範圍0.4 µM ~ 50 µM和 1 ~ 150 μM。

第三部份利用聚吡咯(PPy)、石墨烯(rGO)及酵素GOD以電化學方式聚合同時將其沉積GCE上作為葡萄糖感測器之應用。利用原子力顯微鏡(AFM)與場發射掃描式電子顯微鏡(FE-SEM)觀察酵素是否確實同時沉積於電極表面上。PPy/rGO奈米複合薄膜對於過氧化氫具有較高的訊號且呈線性比例。利用安培法以PPy/rGO/GOD奈米複合薄膜偵測葡萄糖濃度,所得到靈敏度為332.80 nA/mM cm2,線性範圍0.5~30 mM,應答時間約為8~12秒。並由干擾物實驗證實此葡萄糖感測器可避免抗壞血酸及尿素干擾,並成功將PPy/rGO/GOD奈米複合薄膜用來偵測合成血清中的葡萄糖。

A noncovalent methd was used to diaperse graphene (rGO) into Nafion aqueous solution. The efficient electrode for electrocatalytic detection of acetaminophen and aspirin can be directly obtained. The morphology of resulting rGO nanocomposite was characterized by field emission scanning electron microscopy (FE-SEM). Cyclic voltammetry and square-wave voltammetry were used to investigate the electrochemical behavior of acetaminophen and aspirin at rGO/Nafion/GCE. Compared to a bare GCE, the rGO/Nafion coated GCE exhibited electrocatalytic activity and the ability to promote electron trandfer. The determination of aspirin with square-wave voltammetry displayed a sensitivity of 3.521 AM−1 cm−2 and concentration range from 1 - 150 μM; the sensitivity of acetaminophen was 50.77 AM−1 cm-2 and the concentration range from 0.3 - 60 μM with the correlation coefficient of 0.994 using square-wave voltammetry. The rGO/Nafion coated GCE shows excellent sensitivity for the detection of aspirin and acetaminophen, thus it is promising for the future development of electrochemical sensors.
In the next part, this study was to investigate a one-step procedure for fabricating enzyme glucose sensor. The nanobiocomposite film of polypyrrole (PPy), reduced graphene oxide (rGO), and glucose oxidase (GOx) simultaneously deposited on a glassy carbon electrode (GCE) by performing electropolymerization. Detecting hydrogen peroxide of the PPy/rGO nanocomposite film proportionately yielded an amperometric response. This result indicates that the PPy/rGO/GOx biosensor generated a current response when detecting glucose in the solution under the optimal condition. To compare the morphology with the absence and presence of GOx in PPy/rGO nanocomposite film using atomic force microscopy (AFM) and scanning electron microscopy (SEM).The optimal glucose biosensor displayed a wide linear range from 0.5 to 30 mM, a sensiitivity of 332.8 nAmM-1cm-2, and a response time of less than 12 s.This biosensor exhibited favorable anti-interference property and it is suitable for application in the determination of glucose in synthetic serum.
其他識別: U0005-0907201314151100
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