臺灣博碩士論文加值系統

生物感測器目前在醫學檢測上已經有極大的幫助。其中葡萄糖感測器已成為方便且成熟之檢測用品，全世界每年之消耗量極為龐大，使此產品極具有經濟價值。本研究中為了製備低成本之金電極葡萄糖感測器，先使用含鈀觸媒之油墨利用網印方式作為基板，探討其硬度及鈀觸媒含量的影響。再來製作特別的反應槽，採用化學電鍍的方式將鎳、鈀及金三種金屬分別鍍在基板之上，最終目的使其增加產品對血液之導電性。化學電鍍方面，比較溫度、時間、金屬硬度及厚度對產品穩定性之影響。之後在金金屬表面點上酵素，比較使用金電極與其他市售碳電極葡萄糖感測器等之差異以及準確度。最後將之放大量化作業，使其更加擁有商業價值。研究中以聚焦離子束與電子束顯微鏡(FIB)、掃描式電子顯微鏡(SEM)和化學分析電子儀(XPS)等儀器鑑定產品之物理、化學特性和表面性質。結果顯示：鎳鈀金三個反應槽在特定的溫度與時間區間中會有較好的化學鍍品質，最終測試的結果發現鎳的厚度在極薄的情況下整體的準確度會上升達到工業需求的標準。並且金電極所做出之葡萄糖感測器，測出之準確性較其他電極良好，可積極用於市面上。

With the rapid development of technology, biosensors have been used extensively in medical detecting. Glucose biosensors, which have become the convenient and mature product, have great economic value because of huge consume in the world. In this study, in order to prepare lower cost gold electrode glucose biosensors, the screen printed substrate which contained palladium catalyst was prepared. The effects of contents of palladium on the performance of biosensor was investigated. A reactor for electroless plating was designed. Nickel, palladium and gold were deposited on the substrate in order to increase the conductivity of electron passed through the sample. The operating parameters such as temperature, time, hardness and thickness were changed to study their effects on the stability of product. The samples were then doped by the enzyme to check the performance of glucose biosensors. The samples were characterized by focused ion beam (FIB), scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The results illustrated that the better operating conditions of electroless reactors for nickel, palladium and gold was at the region of temperature and dipping time.

摘要 i
Abstract ii
Table of content iii
List of Figures v
List of Tables vii
CHAPTER 1 INTRODUCTION 1
CHAPTER 2 LITERATURE REVIEW 5
2.1 Development of Glucose Biosensors 5
2.1.1 The first generation glucose biosensors 5
2.1.2 The second generation glucose biosensors 6
2.1.3 The third generation glucose biosensors 7
2.2 Electrode 7
2.2.1 Carbon electrode 8
2.2.2 Carbon nanotube electrode 10
2.2.3 Nanosized SiO2 film on Pt electrode 11
2.2.4 Gold nanoparticles electrode 13
2.3 Enzyme 14
2.4 Objective 16
CHAPTER 3 EXPERIMENTAL 18
3.1 Chemicals 18
3.2 Preparation of Solution 18
3.2.1 Preparation of reducing and pickling solution 18
3.2.2 Preparation of nickel solution 18
3.2.3 Preparation of palladium solution 19
3.2.4 Preparation of gold solution 19
3.3 The Characterization of Samples 20
3.3.1 X-ray photoelectron spectroscopy (XPS) 20
3.3.2 Focused ion beam (FIB) 21
3.3.3 Optical microscope (OM) 22
3.3.4 100 grid knives and pencil testers 23
3.4 Reaction Steps 24
CHAPTER 4 RESULT and DISCUSSION 26
4.1 The Characterize of Substrate 26
4.1.1 XPS 26
4.1.2 Hardness 28
4.2 The Result of Electroless Plating 30
4.2.1 The variety of temperature and time 30
4.2.2 OM 35
4.2.3 FIB 36
4.2.4 XPS 40
4.2.5 Hardness 43
4.3 The Consequent of Final Product 43
CHAPTER 5 CONCLUSIONS 47
References 49

Albareda-Sirvent, M., and A. L. Hart. "Preliminary estimates of lactic and malic acid in wine using electrodes printed from inks containing sol–gel precursors."Sensors and Actuators B: Chemical 87.1 (2002): 73-81.

Bakker, E. "Electrochemical sensors." Analytical chemistry 76.12 (2004): 3285-3298.

Bartlett, P. N., and R. G. Whitaker. "Electrochemical immobilisation of enzymes: Part II. Glucose oxidase immobilised in poly-N-methylpyrrole."Journal of electroanalytical chemistry and interfacial electrochemistry 224.1 (1987): 37-48.

Biscay, Julien, et al. "Enzymatic Sensor Using Mediator‐Screen‐Printed Carbon Electrodes." Electroanalysis 23.1 (2011): 209-214.

Chiu, Jing-Yang, et al. "Glucose sensing electrodes based on a poly (3, 4-ethylenedioxythiophene)/Prussian blue bilayer and multi-walled carbon nanotubes." Biosensors and Bioelectronics 24.7 (2009): 2015-2020.

Crouch, Eric, et al. "A novel, disposable, screen-printed amperometric biosensor for glucose in serum fabricated using a water-based carbon ink."Biosensors and Bioelectronics 21.5 (2005): 712-718.

Du, Ying, et al. "A simple method to fabricate a chitosan-gold nanoparticles film and its application in glucose biosensor." Bioelectrochemistry 70.2 (2007): 342-347.

Ghica, Mariana Emilia, and Christopher MA Brett. "A glucose biosensor using methyl viologen redox mediator on carbon film electrodes." Analytica Chimica Acta 532.2 (2005): 145-151.

Gonzalo-Ruiz, Javier, M. Asunción Alonso-Lomillo, and F. Javier Munoz. "Screen-printed biosensors for glucose determination in grape juice."Biosensors and Bioelectronics 22.7 (2007): 1517-1521.

Gorton, Lo. "A carbon electrode sputtered with palladium and gold for the amperometric detection of hydrogen peroxide." Analytica Chimica Acta 178 (1985): 247-253.

Guan, Wen-Jun, et al. "Glucose biosensor based on multi-wall carbon nanotubes and screen printed carbon electrodes." Biosensors and Bioelectronics 21.3 (2005): 508-512.

Hashim, A. J., et al. "Structural and Optical Properties of Zinc Oxide Film Prepared Using RF-Sputtering Technique for Glugose Biosensor." Int. J. Electrochem. Sci 7 (2012): 11876-11883.

Kumar, Satish, et al. "Synthesis, Structure, and Properties of PBO/SWNT Composites&." Macromolecules 35.24 (2002): 9039-9043.

Liu, Haiping, et al. "Gold Immersion Deposition on Electroless Nickel Substrates Deposition Process and Influence Factor Analysis." Journal of The Electrochemical Society 154.12 (2007): D662-D668.

Malitesta, Cosimino, et al. "Glucose fast-response amperometric sensor based on glucose oxidase immobilized in an electropolymerized poly (o-phenylenediamine) film." Analytical Chemistry 62.24 (1990): 2735-2740.

Muguruma, Hitoshi, Tatsuya Hoshino, and Kohei Nowaki. "Electronically type-sorted carbon nanotube-based electrochemical biosensors with glucose oxidase and dehydrogenase." ACS applied materials & interfaces 7.1 (2014): 584-592.

Palmisano, Francesco, et al. "A disposable, reagentless, third-generation glucose biosensor based on overoxidized poly (pyrrole)/ tetrathiafulvalene- tetracyanoquinodimethane composite." Analytical chemistry 74.23 (2002): 5913-5918.

Petukhov, I. V. "Of the mechanism governing the growth of electrolessly deposited nickel-phosphorus coatings." Russian Journal of Electrochemistry43.1 (2007): 34-41.

Rohm, Ingrid, et al. "Development of ultraviolet-polymerizable enzyme pastes: bioprocess applications of screen-printed L-lactate sensors." Analyst 121.6 (1996): 877-881.

Sasso, Sophie, et al. "Thermal denaturation of bacterial and bovine dihydrofolate reductases and their complexes with NADPH, trimethoprim and methotrexate." Journal of Biomolecular Structure and Dynamics 12.5 (1995): 1023-1032.

Wang, Jianwen, et al. "Disposable biosensor based on immobilization of glucose oxidase at gold nanoparticles electrodeposited on indium tin oxide electrode." Sensors and Actuators B: Chemical 135.1 (2008): 283-288.

Wang, Joseph. "Electrochemical glucose biosensors." Chemical reviews 108.2 (2008): 814-825.

Wang, Joseph. "Glucose biosensors: 40 years of advances and challenges."Electroanalysis 13.12 (2001): 983.

Yakobson, Boris I., and Richard E. Smalley. "Fullerene nanotubes: C 1,000,000 and beyond: Some unusual new molecules—long, hollow fibers with tantalizing electronic and mechanical properties—have joined diamonds and graphite in the carbon family." American Scientist 85.4 (1997): 324-337.

Yang, Haipeng, and Yongfa Zhu. "A high performance glucose biosensor enhanced via nanosized SiO 2." Analytica Chimica Acta 554.1 (2005): 92-97.

Zhang, Yuesheng, et al. "Anticarcinogenic activities of sulforaphane and structurally related synthetic norbornyl isothiocyanates." Proceedings of the National Academy of Sciences 91.8 (1994): 3147-3150.