奈米銥修飾之還原態氧化石墨烯於電化學式葡萄糖感測器之應用

Preparation of Iridium Nanoparticles Decorated Reduced Graphene Oxide and the Application of Glucose Biosensors

楊政輯(Cheng-Chi-Yang)

指導教授 ： 王詩涵

義守大學/理工學院/化學工程學系暨生物技術與化學工程研究所/碩士(2015年)

https://doi.org/10.6343/ISU.2015.00324

摘要

由於慢性疾病日漸頻繁，若能及早發現及早治療，對於其治癒率及預後狀況皆有幫助，於疾病早期生物標誌濃度皆低，因此發展極低濃度之感測技術為一重要課題。因此過氧化氫的檢測十分重要，其廣泛使用於臨床醫療、食品、工業製程、環境監測等領域上，因為大部分氧化酶之產物且具電活性，因此為重要的標的物。使用電化學式生物感測器感測過氧化氫，具有價格低廉、檢測時間短與靈敏度高等優點。
本研究結合超臨界水熱法合成銥金屬奈米粒子與RGO之特殊電性及物理性質，製備出Ir / RGO複合材料。運用X射線光電子能譜儀(XPS)、穿透式電子顯微鏡(TEM)、傅利葉紅外線光譜儀(FTIR)研究材料表面結構研究結果顯示，因以超臨界水具有無表面張力之特性，所製備出超微粒銥奈米粒子均勻分布在RGO表面其粒徑約為0.5 - 1.5 nm之間。
利用電化學系統以循環伏安法(CV)與差式脈波伏安法(DPV)對於H2O2濃度量測，Ir/ RGO複合材料具有低氧化電位約為0.16 V ，並可以量測濃度110-4 - 110-19 M之過氧化氫，本研究成功地建立極低濃度過氧化氫電化學感測平台技術。
最終目的是發展出葡萄糖生物感測器將葡萄糖氧化酶固定化於電極表面上，進行葡萄糖之電化學檢測。其酵素電極表現出檢測範圍與最低檢測極限分別為10-100 fM 和5.36 μA fM −1 cm −2 用於測量極低濃度葡萄糖同時具有較高的靈敏度以及良好的再現性，感測系統不會受到pH值顯著的影響皆具有穩定氧化電流，本研究成功地建立極低濃度(fM)葡萄糖電化學感測平台技術。

關鍵字

超臨界流體技術 ； 銥奈米金屬 ； 還原態氧化石墨烯 ； 電化學式感測器 ； 葡萄糖生物感測器

並列摘要

It is important to detect the relative low for early stage chronic or epidemic diseases. It is crucial to develop more sensitive, rapid, user friendly and less expensive methods. Among various bioanalytic techniques, electrochemical method is a potential method. In addition, hydrogen peroxide based analysis plays an important role especially for the enzymatic reactions. In this study, a intensely sensitive electrochemical sensor based on iridium nanoparticles for the rapid and accurate estimation of H2O2 by electrooxidation in physiological conditions is reported. Iridium NPs-decorated reduced graphene oxide nanocatalysts (Ir/RGO) were prepared by hydrothermal technique. The surface and chemical properties were characterized by TEM with HAADF detector and XPS. The particle size of the decorated iridium in supercritical condition was around 0.5 nm-1.5 nm and the distribution was uniform. Cyclic voltammetry characterization measurements, the Ir/RGO catalyzed the oxidation reaction to lower the oxidation potential to around 0.16 V. In order to simplified the sensing process and eliminated the background current, the differential potential voltammetry was applied for the further sensing for the lower concentration range. The experimental result represented that the detection limit could be lower to 0.1 fM. This electrode was also applied for glucose sensing after immobilizing glucose oxidase onto the electrode. The developed biosensor exhibits excellent sensitivity towards glucose over a wide linear range of 10-100 fM with a sensitivity of 5.36 μA fM −1 cm −2 . There was no significant pH effect in this sensing system. In other words, an ultrasensitive sensor for femto-molar-level glucose detection was successfully developed.

並列關鍵字

Hydrothermal technique ； iridium metal nanoparticles ； reduced grapheme oxide ； electrochemical sensor ； glucose biosensor

參考文獻

[29] 吳宗遠，生物感測器：原理與應用之簡介，化學 七十一卷第三期，pp253-264，2013。

[37] 游源祥,石墨烯/高分子奈米複合材料,輔仁大學化學系,化學第七十卷第一期53-67頁，2012。

[4] C. Shan, H. Yang, D. Han, Q. Zhang, A. Iva , N. Li , Graphene /AuNPs /chitosan nanocomposites film for glucose biosensing , Biosensors and Bioelectronics , 25, 2010, pp. 1070-1074.

[10] T. Yin, W. Qin , Applications of nanomaterials in potentiometric sensors ,Trends in Analytical Chemistry , 51, 2013, pp. 79-86.

[13] 李世光，郭宜靜，黎凱強，張谷寧，陳菁菘，陳盈樺，李世元，陳品龍，以導電連結分子為基礎之免標定阻抗式生物感測器,化學第六十九卷第三期pp.193-198頁。