臺灣博碩士論文加值系統

本論文藉由網版印刷技術(Screen-Printed Technology)、射頻濺鍍系統(Radio Frequency Sputtering System)、熱蒸鍍系統(Thermal Evaporation System)將氧化銦鎵鋅(Indium Gallium Zinc Oxide, IGZO)、鋁電極、銀膠導線整合於可撓式基板，爾後，再以共價鍵結法將抗壞血酸氧化酶(Ascorbate Oxidase, AOX)固化於感測膜上，將此元件備製成一可撓式陣列型氧化銦鎵鋅之抗壞血酸生醫感測器。此外本論文利用氧化石墨烯(Graphene Oxide, GO)及磁珠(Magnetic Beads, MBs)修飾氧化銦鎵鋅之感測膜，藉此提高酵素之固化能力與感測器之感測特性，且使用電化學阻抗分析儀(Electrochemical Impedance Spectroscopy, EIS)確認氧化石墨烯與磁珠是否成功修飾於感測膜上。根據實驗結果，此經由氧化石墨烯與磁珠修飾之抗壞血酸生醫感測器之感測度與線性度分別為78.9 mV/decade與0.997。本論文亦探討感測器之響應時間、時漂、遲滯、抗干擾與生命週期等特性。此外，本論文亦使用微流體架構整合此感測器測量感測器於不同流速下之感測特性。最後將此感測器結合以XBee模組建立之無線量測系統為實現無線遠端之偵測。

In this thesis, the screen-printed technology, radio frequency sputtering system and thermal evaporation system were used to integrate indium gallium zinc oxide (IGZO) membrane, Al electrode and silver paste onto the PET (polyethylene terephthalate) substrate. Next, the covalent bonding was used to immobilize ascorbate oxidase (AOX) onto the IGZO sensing membrane, and the flexible arrayed enzymatic L-ascorbic acid (L-AA) biosensor was completed. Besides, the graphene oxide (GO) and magnetic beads (MBs) were used to modify IGZO sensing membrane, and the electrochemical impedance spectroscopy (EIS) was used to confirm whether the GO and MBs were modified onto the sensing membrane successfully. According to the experimental results, the average sensitivity and linearity of MBs-AOX/GO/IGZO/Al L-AA biosensor were 78.9 mV/decade and 0.997, respectively. In this thesis, the response time, drift effect, hysteresis effect, anti-interfering effect and life time were investigated. Moreover, the sensing characteristic of L-AA biosensor which was integrated with microfluidic framework was detected under the different flow rates. Finally, in order to achieve remote monitoring, the L-AA biosensor was integrated with wireless real-time sensing system based on XBee module.

摘要 i
ABSTRACT ii
誌謝 iii
Contents iv
List of Tables ix
List of Figures x
Chapter 1 Background 1
1.1 Introduction 1
1.2 Motive and Purpose 7
1.3 Thesis Outline 11
Fig. 1-1 The flow chart in this thesis. 13
Chapter 2 Introduction 14
2.1 Sensing Materials 14
2.1.1 Indium Gallium Zinc Oxide 15
2.1.2 Graphene Oxide 16
2.1.3 Magenetic Beads 17
2.2 Electrochemical Sensor 19
2.2.1 Sensing Theory of Electrochemical Sensor 19
2.2.2 Sensing Characteristics of Electrochemical Sensor 22
2.3 Enzymatic Biosensor 29
2.3.1 Enzyme and Immobilization 29
2.3.2 Reaction Mechanism of Enzymatic L-AA Biosensor 32
2.4 Measurement System 34
2.4.1 Voltage-Time Measurement System 34
2.4.2 Microfluidic Measurement System 35
2.4.3 Wireless Real-Time Sensing System 36
2.4.4 Electrochemical Impedance Spectroscopy 37
Chapter 3 Experimental 45
3.1 Materials and Instruments 45
3.2 Fabrication of Flexible Arrayed L-AA Biosensors 48
3.2.1 L-AA Biosensors Based on IGZO/Al Membrane 48
3.2.2 L-AA Biosensors Based on GO/IGZO/Al Membrane 49
3.2.3 L-AA Biosensors Based on MBs/GO/IGZO/Al Membrane 51
3.3 Monitoring under Static and Dynamic Test Solutions 53
3.4 Analysis of Electrochemical Impedance Spectroscopy 54
3.5 Remote Monitoring Using Wireless Real-Time Sensing System 55
Chapter 4 Results and Discussion 60
4.1 Analysis of Flexible Arrayed L-AA Biosensor 60
4.1.1 Characterization of L-AA Biosensors Based on IGZO/Al Membrane under Static L-AA Solutions 60
4.1.2 Drift Effect of L-AA Biosensor Based on IGZO/Al Membrane 61
4.1.3 Hysteresis Effect of L-AA Biosensor Based on IGZO/Al Membrane 62
4.1.4 Electrochemical Impedances of IGZO/Al Membrane 63
4.1.5 Response Time of L-AA Biosensor Based on IGZO/Al Membrane 64
4.2 Analysis of Flexible Arrayed L-AA Biosensor Based on GO/IGZO/Al Membrane 66
4.2.1 Characterization of L-AA Biosensors Based on IGZO/Al Membrane under Static L-AA Solutions 66
4.2.2 Drift Effect of L-AA Biosensor Based on GO/IGZO/Al Membrane 68
4.2.3 Hysteresis Effect of L-AA Biosensor Based on GO/IGZO/Al Membrane 69
4.2.4 Electrochemical Impedances of GO/IGZO/Al Membrane 69
4.2.5 Response Time of L-AA Biosensor Based on GO/IGZO/Al Membrane 70
4.2.6 Interference Effect of L-AA Biosensor Based on IGZO/Al Membrane 71
4.2.7 pH Effect for Average Sensitivity of L-AA Biosensor 72
4.2.8 Detection Limit of L-AA Biosensor Based on GO/IGZO/Al Membrane 73
4.3 Analysis of Flexible Arrayed L-AA Biosensor Based on MBs/GO/IGZO/Al Membrane 74
4.3.1 Characterization of L-AA Biosensors Based on IGZO/Al Membrane Modified by GO and MBs under Static and Dynamic L-AA Solutions 74
4.3.2 Drift Effect of L-AA Biosensor Based on MBs/GO/IGZO/Al Membrane 76
4.3.3 Hysteresis Effect of L-AA Biosensor Based on MBs/GO/IGZO/Al Membrane 77
4.3.4 Electrochemical Impedances of MBs/GO/IGZO/Al Membrane 77
4.3.5 Response Time of L-AA Biosensor Based on MBs/GO/IGZO/Al Membrane 78
4.3.6 Interference Effect of L-AA Biosensor Based on MBs/GO/IGZO/Al Membrane 79
4.3.7 Detection Limit of L-AA Biosensor Based on GO/IGZO/Al Membrane 80
4.3.8 Temperature Effect of L-AA Biosensor Based on MBs/GO/IGZO/Al Membrane 81
4.4 Comparisons with Sensing Characteristic for Various L-AA Biosensors 83
4.5 Comparisons with Electrochemical Impedances of Different Membranes 87
4.6 Lifetime and Decay Rate of MBs/GO/IGZO/Al L-AA Biosensor 90
4.7 Surfaces of IGZO and GO Membranes Characterized via Field Emission Scanning Electronic Microscope 92
4.8 Specific Surface Areas of IGZO Membrane and GO Membrane 93
4.9 Surface Roughness for IGZO/Al, GO/IGZO/Al and MB/GO/IGZO/Al Membranes 94
4.10 Analysis of Remote Monitoring for L-AA Biosensor 95
4.11 Specifications of IGZO/Al-based L-AA biosensor 96
Chapter 5 Conclusions 143
Chapter 6 Future Work 148
References 149
Appendix I: 175
1. 許渭州 委員 175
2. 廖義宏 委員 177
3. 周學韜 委員 181
4. 賴志賢 委員 182
5. 周榮泉 委員 186

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