研究生: |
翟祐暄 You-syuan Jhai |
---|---|
論文名稱: |
以二十四面奈米金屬觸媒修飾製備電流式雙氧水感測器與其應用 Fabrication of Amperometric Hydrogen Peroxide Biosensor Based on Trisoctahedral Nano-Metallic Catalyst and its Applications |
指導教授: |
王孟菊
Meng-jiy Wang |
口試委員: |
王文
Wen Wang 黃炳照 Bing-joe Hwang 林俊成 Jing-cheng Lin 郭俞麟 Yu-lin Kuo |
學位類別: |
碩士 Master |
系所名稱: |
工程學院 - 化學工程系 Department of Chemical Engineering |
論文出版年: | 2012 |
畢業學年度: | 100 |
語文別: | 中文 |
論文頁數: | 131 |
中文關鍵詞: | 核殼式 、奈米金屬觸媒 、雙氧水氧化反應 、葡萄糖 、生物感測器 |
外文關鍵詞: | Nano-metallic catalyst, Oxidation of hydrogen peroxide |
相關次數: | 點閱:259 下載:1 |
分享至: |
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本研究論文中將研究分為兩部分:(I) 二十四面體奈米金結晶(trisoctahedral gold nanocrystal, AuNCs)與核殻(core-shell)奈米金鉑(AuNCs@Pt)之合成與其電化學觸媒應用於催化雙氧水氧化還原反應感測分析。(II) 以交聯架橋法結合吸附方法固定酵素分子製備之葡萄糖生物感測器應用。
首先,研究中第一部份將探討合成出的奈米金結晶與奈米鉑-金結晶之表面形態特性與晶相組成,及利用電化學法進行雙氧水感測與分析,因奈米金結晶具有多邊角結構而擁有眾多活性位置,為了再進一步提高奈米金屬觸媒的活性,在其表面上合成奈米鉑粒子,形成以少量鉑合成出之多面體奈米鉑結晶。由掃描式電子顯微鏡觀測鉑還原於奈米金表面,再利用紫外光-可見光光譜 (UV-vis) 及電化學酸處理結果確認鉑還原於奈米金表面,達成核殼式的奈米金鉑結構,之外,亦與玻璃碳、塊材金及市售鉑奈米觸媒比較催化雙氧水情形,並使用不同之驅動電壓與不同Nafion濃度找出最佳之感測狀態為0.5 V、0.5% Nafion,在此最佳雙氧水感測狀態表現出低偵測極限10 μM,合適線性範圍0.01 - 5.1 mM (R2 = 0.997),優秀的靈敏度397.37 μA/mM cm2,且擁有良好抗干擾能力之雙氧水感測電極。
本論文研究中第二部份,為將雙氧水感測器應用於氧化酶感測器,建立最適化電極感測層之結構,利用奈米金結晶與蛋白質酵素混合吸附固定後,再添加微量交聯劑幫助酵素間進行交聯反應,找尋酵素溶液配方活性單位最佳量,此酵素固定化所製備之酵素感測器不僅提供溫和環境固定酵素於電極表面,修飾之離子薄膜幫助酵素與待測物質間進行選擇性生物反應,使酵素具有良好之親合性與穩定性。本研究所製備之葡萄糖感測器於0.5 V v.s Ag/AgCl施加電位下,具有感測葡萄糖線性範圍為1.0 - 7.01 mM (R2=0.996),且其偵測靈敏度86.93 μA/mMcm2,結果顯示,藉由合成之雙元奈米金屬觸媒搭配交聯結合吸附法應用於生物感測器之製程系統,成功製備具優良再現性與量測準確度、高靈敏度葡萄糖感測電極。
This study was comprised of two parts: (I) the synthesis of trisoctahedral gold nanocrystal (AuNC) and core-shell AuNCs@Pt catalysts for the applications of electrochemical sensing of hydrogen peroxide; (II) the immobilization of enzymatic species by adding cross-linking agent to fabricate electrochemical glucose sensor.
For the first part, the surface morphology and crystal lattice of the synthesized nano-metallic catalysts were investigated using SEM, XRD. The synthesized AuNCs showed many active sites due to their polyhedral structure. In order to enhance the catalytic ability, the AuNCs with outer layer of platinum (to form polyhedral nano platinum crystals) was synthesized which provides a particular advantage of only a small amout of platinum was needed. The results of UV-vis spectropy and electrochemical acid treatment showed that the bimetallic catalyst is core-shell structure which was almost completely covered by reduced platinum. The detection of hydrogen peroxide was measured by electrochemical methods. Moreoer, the optimized parameters for electrochemical analyses including the applied voltage and the surface protection layer were applied for the detection of hydrogen peroxide. The results showed that the detection limit of 10 μM, with a linear range of detection from 0.01 to 5.1 mM (R2=0.997), high sensitivity of 397.37 μA/(mMcm2), and excellent anti-interfering ability were obtained for the prepared sensing system.
For the second part, the prepared sensing layer on the electrodes was further applied for the detection of glucose. In this study, the synthesized AuNCs were used to adsorb enzyme molecules which were followed by the addition of cross-linking agent to ensure the combination. The enzyme loading and operating parameters were optimized. It showed that the assembled sensor prepared under the optimized condition provided mild environment for enzyme immobilization and facilitated the bio-reaction between enzyme and bio-species, which allowed enzyme exhibiting good affinity and stability. The obtained glucose sensing at 0.5 V v.s Ag/AgCl applied potential showed linear range of 1.0 to 7.0 mM (R2=0.996), with sensitivity of 86.93 μA/mMcm2. We have shown that a highly sensitive glucose biosensor with good reproducibility and precision, high sensitivity, and great stability was successfully prepared.
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