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  1. NTU Theses and Dissertations Repository
  2. 工學院
  3. 材料科學與工程學系
請用此 Handle URI 來引用此文件: http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/69330
完整後設資料紀錄
DC 欄位值語言
dc.contributor.advisor羅世強
dc.contributor.authorPo-chun Huangen
dc.contributor.author黃柏鈞zh_TW
dc.date.accessioned2021-06-17T03:13:04Z-
dc.date.available2019-07-19
dc.date.copyright2018-07-19
dc.date.issued2018
dc.date.submitted2018-07-12
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21. Chen, C. H.; Luo, S. C., Tuning Surface Charge and Morphology for the Efficient Detection of Dopamine under the Interferences of Uric Acid, Ascorbic Acid, and Protein Adsorption. Acs Applied Materials & Interfaces 2015, 7 (39), 21931-21938.
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25. Luo, S. C., Conducting Polymers as Biointerfaces and Biomaterials: A Perspective for a Special Issue of Polymer Reviews. Polymer Reviews 2013, 53 (3), 303-310.
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27. Zhu, B.; Luo, S. C.; Zhao, H. C.; Lin, H. A.; Sekine, J.; Nakao, A.; Chen, C.; Yamashita, Y.; Yu, H. H., Large enhancement in neurite outgrowth on a cell membrane-mimicking conducting polymer. Nature Communications 2014, 5.
28. Guan, Y.; Zhang, Y., Boronic acid-containing hydrogels: synthesis and their applications. Chemical Society Reviews 2013, 42 (20), 8106-8121.
29. Mader, H. S.; Wolfbeis, O. S., Boronic acid based probes for microdetermination of saccharides and glycosylated biomolecules. Microchimica Acta 2008, 162 (1-2), 1-34.
30. Gamsey, S.; Suri, J. T.; Wessling, R. A.; Singaram, B., Continuous glucose detection using boronic acid-substituted viologens in fluorescent hydrogels: linker effects and extension to fiber optics. Langmuir 2006, 22 (21), 9067-9074.
31. Zhong, X.; Bai, H. J.; Xu, J. J.; Chen, H. Y.; Zhu, Y. H., A Reusable Interface Constructed by 3‐Aminophenylboronic Acid‐Functionalized Multiwalled Carbon Nanotubes for Cell Capture, Release, and Cytosensing. Advanced Functional Materials 2010, 20 (6), 992-999.
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36. Stephenson-Brown, A.; Wang, H. C.; Iqbal, P.; Preece, J. A.; Long, Y. T.; Fossey, J. S.; James, T. D.; Mendes, P. M., Glucose selective Surface Plasmon Resonance-based bis-boronic acid sensor. Analyst 2013, 138 (23), 7140-7145.
37. Kajisa, T.; Sakata, T., Glucose-responsive hydrogel electrode for biocompatible glucose transistor. Science and Technology of Advanced Materials 2017, 18 (1), 26-33.
38. Kajisa, T.; Sakata, T., Fundamental Properties of Phenylboronic-Acid-Coated Gate Field-Effect Transistor for Saccharide Sensing. Chemelectrochem 2014, 1 (10), 1647-1655.
39. Sugnaux, C.; Klok, H. A., Glucose-Sensitive QCM-Sensors Via Direct Surface RAFT Polymerization. Macromolecular Rapid Communications 2014, 35 (16), 1402-1407.
40. Zhai, W. L.; Sun, X. L.; James, T. D.; Fossey, J. S., Boronic Acid-Based Carbohydrate Sensing. Chemistry-an Asian Journal 2015, 10 (9), 1836-1848.
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42. Nishiyabu, R.; Kubo, Y.; James, T. D.; Fossey, J. S., Boronic acid building blocks: tools for self assembly. Chemical Communications 2011, 47 (4), 1124-1150.
43. Egawa, Y.; Miki, R.; Seki, T., Colorimetric sugar sensing using boronic acid-substituted azobenzenes. Materials 2014, 7 (2), 1201-1220.
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45. Huang, R.; Yi, P.; Tang, Y., Probing the interactions of organic molecules, nanomaterials, and microbes with solid surfaces using quartz crystal microbalances: methodology, advantages, and limitations. Environmental Science: Processes & Impacts 2017, 19 (6), 793-811.
46. Reviakine, I.; Johannsmann, D.; Richter, R. P., Hearing what you cannot see and visualizing what you hear: interpreting quartz crystal microbalance data from solvated interfaces. ACS Publications: 2011.
47. Macdonald, D. D., Reflections on the history of electrochemical impedance spectroscopy. Electrochimica Acta 2006, 51 (8-9), 1376-1388.
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49. Ning, C.; Segal, S., Plasma galactose and galactitol concentration in patients with galactose-1-phosphate uridyltransferase deficiency galactosemia: Determination by gas chromatography /mass spectrometry. Metabolism-Clinical and Experimental 2000, 49 (11), 1460-1466.
dc.identifier.urihttp://tdr.lib.ntu.edu.tw/jspui/handle/123456789/69330-
dc.description.abstract1957年,發明了第一個葡萄糖感測器主要是利用葡萄糖氧化酶(glucose oxidase)來修飾電極並且利用過氧化氫的氧化還原來偵測葡萄糖,但是傳統利用酶的葡萄糖感測器易因為環境因素而使得偵測失真。隨著科技的進步,新型的葡萄糖感測器則是使用化學分子來取代酶當作葡萄糖的受體。本實驗最主要利用含有硼酸的導電高分子薄膜來製作出非酶的葡萄糖感測器,希望未來可應用於長時間血糖監控系統。根據以前的文獻表示硼酸(boronic acid)可以乙二醇形成可逆的共價鍵結,而在鹼性的環境中,硼酸對乙二醇的吸引力會變更大。由上述所知硼酸的官能基非常適合用來當作血糖感測器的受體。我們將合成的方式將3,4-乙烯二氧基噻吩 (3,4-ethylenedioxythiophene, EDOT) 和硼酸官能基接上製備成硼酸官能化3,4-乙烯二氧基噻吩(EDOT-PBA)。接著使用電化學聚合的方式將製備出含有硼酸酸官能基的導電高分子薄膜,而且我們利用了不同的製成方式使得導電高分子膜的表面形貌都皆為不同。從二氯甲烷(dichloromethane)所製備出的導電高分子薄膜其表面都是由微小的管狀奈米結構所組成;乙腈和離子液體中所製備出來的表面則是較為平坦。之後我們將在導電高分子薄膜上覆蓋一層牛血清蛋白(BSA)使得表面不但對葡萄糖有特定性吸附又同時有抗沾黏特性避免在有其他的蛋白質或是細菌吸附表面而影響到偵測。我們藉由石英晶體微量天平-耗散偵測系統 (quartz crystal microbalance with dissipation, QCM-D)來觀察葡萄糖和牛血清蛋白的吸附。我們發現導電高分子薄膜的表面形貌會影響到牛血清蛋白和葡萄糖的吸附機制,管狀奈米結構的導電高分子薄膜具有最好的葡萄糖吸附效果還有良好的可逆性,重要的是葡萄糖的吸附不會受到微量的果糖或半乳糖影響。接下來我們使用兩種偵測儀器來觀察導電高分子薄膜對葡萄糖的偵測效果,第一種是石英晶體微量天平-耗散偵測系統其偵測極限在0.5 mM和偵測範圍在0.5 mM ~10 mM 之間;第二種是電化學阻抗頻譜分析(electrochemical impedance spectroscopy)其偵測極限在50 µM和偵測範圍在0.05 mM ~10 mM 之間,並且再利用石英晶體微量天平來做長時間的葡萄糖監控。本實驗證實了含有硼酸官能基的導電高分子薄膜適合應用於血糖感測器並有潛力發展成長時間的血糖偵測系統,其可多次測量而且偵測也不受血液中其他糖類影響。zh_TW
dc.description.abstractIn this study, we have successful demonstrated a nanostructured phenylboronic acid-grafted poly(3,4-ethylenedioxythiophene), poly(EDOT-PBA), platform for fast and sensitive glucose monitoring. The poly(EDOT-PBA) films of well-organized tubular nanostructures can be fabricated by direct electropolymerization without templates. Compared to the smooth poly(EDOT-PBA), the nanotubular poly(EDOT-PBA) shows enhanced glucose sensitivity and different adsorption process of bovine serum albumin (BSA). Besides, the BSA blocking and low concentration fructose and galactose do not affect the sensitivity of this platform. Both quartz crystal microbalance (QCM) and electrochemical impedance spectroscopy (EIS) methods are used and compared for glucose monitoring by applying nanotubular poly(EDOT-PBA) as conductive substrates. Compared to QCM analysis, EIS has higher sensitivity to glucose and the detection limit is about 50 µM. Besides, the poly(EDOT-PBA) film is useful for long-term detecting glucose level by QCM because the binding with glucose on poly(EDOT-PBA) is highly reversibly . Based on these observations, the nanotubular poly(EDOT-PBA) has great potential for enzyme-free electrodes targeting continues glucose monitoring applications.en
dc.description.provenanceMade available in DSpace on 2021-06-17T03:13:04Z (GMT). No. of bitstreams: 1
ntu-107-R05527062-1.pdf: 2310897 bytes, checksum: 69cde080bdc12fa84ed23c2a073ba480 (MD5)
Previous issue date: 2018
en
dc.description.tableofcontents摘要..................................................................................................................................Ⅰ
ABSTRACT...................................................................................................................Ⅲ
CONTENT.....................................................................................................................Ⅳ
FIGURE CAPTIONS....................................................................................................Ⅵ
TABLE CAPTIONS...................................................................................................Ⅷ
CHAPTER 1 CHAPTER 1 INTRODUCTION ......................................................... 1
1.1 Glucose and Diabetes ........................................................................................... 1
1.2 Biosensor ............................................................................................................... 3
1.3 Glucose Sensors .................................................................................................... 4
1.4 Conducting Polymer for Biomaterials ................................................................ 7
1.5 Boronic Acids Functional Group ....................................................................... 10
1.6 Motivation ............................................................................................................ 11
CHAPTER 2 MATERIALS AND METHODS ........................................................ 13
2.1 Materials and Instruments ................................................................................ 13
2.2 Synthesis of EDOT-PBA ..................................................................................... 15
2.3 Electropolymerization of Poly(EDOT-PBA) .................................................... 16
2.4 Surface Characterization of Poly(EDOT-PBA) ............................................... 17
2.4.1 Contact Angle ............................................................................................... 17
2.4.2 Scanning Electron Microscopy (SEM) ....................................................... 17
2.4.3 Atomic Force Microscopy (AFM) ............................................................... 17
2.5 Quartz Crystal Microbalance (QCM) Measurements .................................... 18
2.6 Electrochemistry Impedance Spectroscopy (EIS) Measurements ................. 20
CHAPTER 3 RESULTS AND DISCUSSION .......................................................... 23
3.1 Surface Properties of Poly(EDOT-PBA) Films ................................................ 23
3.1.1 Electropolymerization of Poly(EDOT-PBA) Films ................................... 23
3.1.2 Hydrophilicity .............................................................................................. 26
3.1.3 Morphology, Roughness and Thickness .................................................... 27
3.2 Adsorption of BSA on Poly(EDOT-PBA) Films ............................................... 29
3.3 Adsorption of Glucose on Poly(EDOT-PBA) Films ......................................... 31
3.3.1 Effect of Morphology on Glucose Adsorption ........................................... 31
3.3.2 Effect of pH Value on Glucose Adsorption ................................................ 32
3.3.3 Effect of Interference on Glucose Adsorption ........................................... 34
3.4 The Comparison of Glucose Detection between QCM and EIS Methods ..... 37
3.4.1 Detection Range and Detection Limit ........................................................ 37
3.4.2 Reversible Test ............................................................................................. 41
3.5 Continuous Glucose Monitoring in QCM-D .................................................... 42
CHAPTER 4 CONCLUSION .................................................................................... 44
CHAPTER 5 FUTURE WORKS ................................................................................ 45
REFERENCE ............................................................................................................... 46
dc.language.isoen
dc.subject電化學阻抗頻譜分析zh_TW
dc.subject4-乙烯二氧基?吩zh_TW
dc.subject硼酸官能基zh_TW
dc.subject葡萄糖zh_TW
dc.subject葡萄糖感測器zh_TW
dc.subject石英晶體為天秤zh_TW
dc.subjectGlucoseen
dc.subject4-ethylenedioxythiopheneen
dc.subjectElectrochemistry impedance spectroscopyen
dc.subjectQuartz crystal microbalanceen
dc.subjectBoronic aciden
dc.subjectGlucose sensoren
dc.title"利用苯基硼酸官能基化聚(3,4-乙烯二氧噻吩)作高靈敏又快速偵測的葡萄糖監控系統"zh_TW
dc.titleSurface Engineering of Phenylboronic Acid-Functionalized Poly(3,4-ethylenedioxythiophene) for Fast Responsive and Sensitive Glucose Monitoringen
dc.typeThesis
dc.date.schoolyear106-2
dc.description.degree碩士
dc.contributor.oralexamcommittee陳建甫,康敦彥
dc.subject.keyword3,4-乙烯二氧基?吩,硼酸官能基,葡萄糖,葡萄糖感測器,石英晶體為天秤,電化學阻抗頻譜分析,zh_TW
dc.subject.keyword3,4-ethylenedioxythiophene,Boronic acid,Glucose,Glucose sensor,Quartz crystal microbalance,Electrochemistry impedance spectroscopy,en
dc.relation.page49
dc.identifier.doi10.6342/NTU201800797
dc.rights.note有償授權
dc.date.accepted2018-07-13
dc.contributor.author-college工學院zh_TW
dc.contributor.author-dept材料科學與工程學研究所zh_TW
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