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研究生:高鵬凱
研究生(外文):Peng-Kai Kao
論文名稱:利用電漿製程製備紙為基底之微流道裝置
論文名稱(外文):Fabrication of Microfluidic Paper-based Analytical Devices Using Plasma Processes
指導教授:徐振哲
口試委員:黃駿魏大欽王孟菊
口試日期:2014-07-01
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:化學工程學研究所
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2014
畢業學年度:102
語文別:中文
論文頁數:111
中文關鍵詞:氟碳電漿鍍膜可攜式常壓微電漿產生裝置紙為基底之微流道裝置
外文關鍵詞:fluorocarbon plasma polymerizationportable atmospheric-pressure microplasma generation devicesmicrofluidic paper-based devices on demand
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本研究為利用電漿製程製備以紙為基底之微流道裝置,共提出兩種可行的電漿製程:「單一步驟之氟碳電漿聚合反應」,以及「以電池驅動、可攜式、可撓曲之常壓空氣微電漿蝕刻反應」。第一部分,我們利用單一步驟之氟碳電漿進行聚合反應,其優點包括反應為乾式氣相、快速且解析度良好。藉由FTIR與XPS分析顯示,此製程能於濾紙表面鍍上一疏水性屏障 (氟碳薄膜) 的同時,使紙質微流道和偵測區域的主要化學性質及表面元素鍵結均能維持如未處理的濾紙一般。接著,我們發現電漿製程時間對於所製備之微流體為一關鍵影響因素,當鍍膜時間充足 (例如,180秒),樣品溶液能被完整地侷限在微流體流道內,且在此製程條件下,僅需要4.5 μL之溶液便能完整潤濕一寬度為800 μm之微流道裝置。最後,我們利用亞硝酸鹽檢定顯示此製備方法之可行性。
第二部分,我們提出使用一可攜式微電漿產生裝置 (microplasma generation device, MGD),在常壓下產生空氣電漿進行蝕刻反應以製備紙基微流體。藉由引入製備印刷電路板之碳粉熱轉印法 (toner transfer-based),一輕薄且具可撓性之微電漿產生裝置可於30分鐘內製備完成。此微電漿產生裝置可由一可攜式電源供應器 (重量小於1公斤) 搭配一顆12伏特電池或交流/ 直流轉換器驅動。利用此微電漿產生裝置能進行無遮罩圖案化製程 (maskless patterning),在疏水的紙纖維表面產生微米尺度的親水性圖案,並維持良好的圖案轉移擬真度 (pattern transfer fidelity)。接著,我們利用此微電漿產生裝置製備紙基微流體。在合適的微電漿電極設計之下,能於一分鐘之內、花費小於美金0.05元,製作出一流道寬度500 μm之微流體。最後,我們利用定量比色檢定及繪製檢量線來偵測葡萄糖和亞硝酸鹽,結果顯示葡萄糖和亞硝酸鹽分別於1-50 mM及0.1-5 mM 有線性反應。我們相信此低成本、微小化且可攜式之電漿產生裝置能讓使用者在戶外 (in-field) 以及/或是基於各式需求 (on-demand) 來操作電漿,並應用於各種領域。而以此電漿裝置所製備之微流道裝置可望對生醫分析、環境監控以及食品安全檢驗帶來嶄新發展的可能性。


In this work, we first demonstrated an all-dry, top-down, and one-step rapid process to fabricate paper-based microfluidic devices using fluorocarbon plasma polymerization. This process is able to create fluorocarbon-coated hydrophobic patterns on filter paper substrates while maintaining the trench and detection regions intact and free of contamination after the fabrication process, as confirmed by ATR-FTIR and XPS. We have shown that the processing time is one critical factor that influences the device performance. For the device fabricated with a sufficiently long processing time (180 s), the sample fluid flow can be well confined in the patterned trenches. By testing the device with 800 μm channel width, a sample solution amount as small as 4.5 μL is sufficient to perform the test. NO2&;#8722; assay is also performed and shows that such a device is capable for biochemical analysis.
In the second part of this master thesis, a portable microplasma generation device (MGD) operated in ambient air is introduced for making a microfluidic paper-based analytical device (μPAD) that serves as a primary healthcare platform. By utilizing a printed circuit board fabrication process, a flexible and lightweight MGD can be fabricated within 30 min with ultra low-cost. This MGD can be driven by a portable power supply (less than two pounds), which can be powered using 12V-batteries or AC-DC converters. This MGD is used to perform maskless patterning of hydrophilic patterns with sub-mm spatial resolution on hydrophobic paper substrates with good pattern transfer fidelity. Using this MGD to fabricate μPADs is demonstrated. With a proper design of the MGD electrode geometry, μPADs with 500 μm-wide flow channels can be fabricated within 1 min and with a cost of less than $USD 0.05/device. We then test the μPADs by performing quantitative colorimetric assay tests and establish calibration curve for detection of glucose and nitrite. The results show a linear response to glucose assay for 1-50 mM and nitrite assay for 0.1-5 mM. The low cost, miniaturized, and portable MGD can be used to fabricate μPADs on demand, which is suitable for in-field diagnostic tests. We believe this concept brings impact to the field of biomedical analysis, environmental monitoring, and food safety survey.


誌謝 I
中文摘要 III
ABSTRACT V
目錄 VII
圖目錄 IX
表目錄 XIII
第1章 緒論 1
1.1 前言 1
1.2 研究動機與目標 2
1.3 論文總覽 2
第2章 文獻回顧 3
2.1 低壓氟碳電漿鍍疏水性薄膜 3
2.1.1 超疏水原理及表面遲滯現象 3
2.1.2 低壓電漿技術 8
2.1.3 電漿鍍氟碳膜研究 9
2.2 常壓微電漿系統 14
2.2.1 常壓微電漿之種類 14
2.2.2 常壓微電漿之應用 21
2.3 紙為基底之微流道裝置 25
2.3.1 紙為基底之微流道裝置之原理與種類 25
2.3.2 紙為基底之微流道裝置之檢測技術 32
2.3.3 紙為基底之微流道裝置應用於疾病檢測 38
第3章 實驗設備與架構 44
3.1 低壓電漿系統以及利用氟碳電漿製備紙基微流體 44
3.2 可攜式常壓微電漿系統及其用於製備紙基微流體 47
3.3 比色檢定與影像處理 54
3.3.1 比色檢定 (Colorimetric assays) 54
3.3.2 影像處理 55
3.4 材料性質分析檢測儀器 56
第4章 實驗結果與討論 58
4.1 利用氟碳電漿製備紙為基底之微流道裝置 58
4.1.1 利用低壓氟碳電漿聚合進行紙為基底之親疏水表面工程 58
4.1.2 單一步驟氟碳電漿製程製備紙上疏水圖案 60
4.1.3 微流體裝置之組成性質與表面化學分析 62
4.1.4 製程時間對紙基微流體輸送行為之影響 68
4.1.5 檢定應用:亞硝酸鈉定量分析 72
4.2 利用可攜式常壓微電漿製備紙為基底之微流道裝置 75
4.2.1 碳粉熱轉印法製備可撓曲微電漿產生裝置 75
4.2.2 疏水性紙基板上製備親水性微流道 76
4.2.3 電漿產生裝置之圖案設計與微流道特性 77
4.2.4 電漿操作參數對紙基微流體輸送行為之影響 80
4.2.5 檢定應用:葡萄糖/ 亞硝酸鈉定量分析 84
4.2.6 手繪法製備微電漿產生裝置之電極 88
第5章 結論與未來展望 90
第6章 文獻回顧 91
附錄 104


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77.P. Rattanarat, W. Dungchai, D. Cate, J. Volckens, O. Chailapakul and C. S. Henry, "Multilayer Paper-Based Device for Colorimetric and Electrochemical Quantification of Metals", Analytical Chemistry, 86 (7), 3555-3562 (2014).
78.S. M. Z. Hossain, R. E. Luckham, M. J. McFadden and J. D. Brennan, "Reagentless Bidirectional Lateral Flow Bioactive Paper Sensors for Detection of Pesticides in Beverage and Food Samples", Analytical Chemistry, 81 (21), 9055-9064 (2009).
79.A. K. Yetisen, M. S. Akram and C. R. Lowe, "Paper-based microfluidic point-of-care diagnostic devices", Lab Chip, 13 (12), 2210-2251 (2013).
80.E. Carrilho, A. W. Martinez and G. M. Whitesides, "Understanding Wax Printing: A Simple Micropatterning Process for Paper-Based Microfluidics", Analytical Chemistry, 81 (16), 7091-7095 (2009).
81.Y. Zhang, C. B. Zhou, J. F. Nie, S. W. Le, Q. Qin, F. Liu, Y. P. Li and J. P. Li, "Equipment-Free Quantitative Measurement for Microfluidic Paper-Based Analytical Devices Fabricated Using the Principles of Movable-Type Printing", Analytical Chemistry, 86 (4), 2005-2012 (2014).
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83.J. Olkkonen, K. Lehtinen and T. Erho, "Flexographically Printed Fluidic Structures in Paper", Analytical Chemistry, 82 (24), 10246-10250 (2010).
84.D. A. Bruzewicz, M. Reches and G. M. Whitesides, "Low-cost printing of poly(dimethylsiloxane) barriers to define microchannels in paper", Analytical Chemistry, 80 (9), 3387-3392 (2008).
85.C. L. Cassano and Z. H. Fan, "Laminated paper-based analytical devices (LPAD): fabrication, characterization, and assays", Microfluid Nanofluid, 15 (2), 173-181 (2013).
86.H. Liu and R. M. Crooks, "Paper-Based Electrochemical Sensing Platform with Integral Battery and Electrochromic Read-Out", Analytical Chemistry, 84 (5), 2528-2532 (2012).
87.W. Dungchai, O. Chailapakul and C. S. Henry, "A low-cost, simple, and rapid fabrication method for paper-based microfluidics using wax screen-printing", Analyst, 136 (1), 77-82 (2011).
88.T. Songjaroen, W. Dungchai, O. Chailapakul and W. Laiwattanapaisal, "Novel, simple and low-cost alternative method for fabrication of paper-based microfluidics by wax dipping", Talanta, 85 (5), 2587-2593 (2011).
89.E. W. Washburn, "The dynamics of capillary flow", Phys. Rev., 17 (3), 273-283 (1921).
90.X. Li, J. Tian and W. Shen, "Progress in patterned paper sizing for fabrication of paper-based microfluidic sensors", Cellulose, 17 (3), 649-659 (2010).
91.E. M. Fenton, M. R. Mascarenas, G. P. Lopez and S. S. Sibbett, "Multiplex Lateral-Flow Test Strips Fabricated by Two-Dimensional Shaping", ACS Appl Mater Inter, 1 (1), 124-129 (2009).
92.E. Fu, B. Lutz, P. Kauffman and P. Yager, "Controlled reagent transport in disposable 2D paper networks", Lab Chip, 10 (7), 918-920 (2010).
93.A. W. Martinez, S. T. Phillips and G. M. Whitesides, "Three-dimensional microfluidic devices fabricated in layered paper and tape", Proc. Natl. Acad. Sci. U. S. A., 105 (50), 19606-19611 (2008).
94.G. G. Lewis, M. J. DiTucci, M. S. Baker and S. T. Phillips, "High throughput method for prototyping three-dimensional, paper-based microfluidic devices", Lab Chip, 12 (15), 2630-2633 (2012).
95.S. J. Vella, P. Beattie, R. Cademartiri, A. Laromaine, A. W. Martinez, S. T. Phillips, K. A. Mirica and G. M. Whitesides, "Measuring Markers of Liver Function Using a Micropatterned Paper Device Designed for Blood from a Fingerstick", Analytical Chemistry, 84 (6), 2883-2891 (2012).
96.H. Liu and R. M. Crooks, "Three-Dimensional Paper Microfluidic Devices Assembled Using the Principles of Origami", J. Am. Chem. Soc., 133 (44), 17564-17566 (2011).
97.E. W. Nery and L. T. Kubota, "Sensing approaches on paper-based devices: a review", Anal Bioanal Chem, 405 (24), 7573-7595 (2013).
98.M. S. Li, J. F. Tian, M. Al-Tamimi and W. Shen, "Paper-Based Blood Typing Device That Reports Patient''s Blood Type "in Writing"", Angew Chem Int Edit, 51 (22), 5497-5501 (2012).
99.A. Apilux, W. Dungchai, W. Siangproh, N. Praphairaksit, C. S. Henry and O. Chailapakul, "Lab-on-Paper with Dual Electrochemical/Colorimetric Detection for Simultaneous Determination of Gold and Iron", Analytical Chemistry, 82 (5), 1727-1732 (2010).
100.W. Dungchai, O. Chailapakul and C. S. Henry, "Electrochemical Detection for Paper-Based Microfluidics", Analytical Chemistry, 81 (14), 5821-5826 (2009).
101.S. G. Ge, L. Ge, M. Yan, X. R. Song, J. H. Yu and J. D. Huang, "A disposable paper-based electrochemical sensor with an addressable electrode array for cancer screening", Chem. Commun., 48 (75), 9397-9399 (2012).
102.K. Abe, K. Kotera, K. Suzuki and D. Citterio, "Inkjet-printed paperfluidic immuno-chemical sensing device", Anal Bioanal Chem, 398 (2), 885-893 (2010).
103.E. Fu, T. Liang, P. Spicar-Mihalic, J. Houghtaling, S. Ramachandran and P. Yager, "Two-Dimensional Paper Network Format That Enables Simple Multistep Assays for Use in Low-Resource Settings in the Context of Malaria Antigen Detection", Analytical Chemistry, 84 (10), 4574-4579 (2012).
104.L. Ge, J. X. Yan, X. R. Song, M. Yan, S. G. Ge and J. H. Yu, "Three-dimensional paper-based electrochemiluminescence immunodevice for multiplexed measurement of biomarkers and point-of-care testing", Biomaterials, 33 (4), 1024-1031 (2012).
105.J. L. Delaney, C. F. Hogan, J. Tian and W. Shen, "Electrogenerated Chemiluminescence Detection in Paper-Based Microfluidic Sensors", Analytical Chemistry, 83 (4), 1300-1306 (2011).
106.J. H. Yu, L. Ge, J. D. Huang, S. M. Wang and S. G. Ge, "Microfluidic paper-based chemiluminescence biosensor for simultaneous determination of glucose and uric acid", Lab Chip, 11 (7), 1286-1291 (2011).
107.L. Ge, S. M. Wang, X. R. Song, S. G. Ge and J. H. Yu, "3D Origami-based multifunction-integrated immunodevice: low-cost and multiplexed sandwich chemiluminescence immunoassay on microfluidic paper-based analytical device", Lab Chip, 12 (17), 3150-3158 (2012).
108.C. Klungthong, R. V. Gibbons, B. Thaisomboonsuk, A. Nisalak, S. Kalayanarooj, V. Thirawuth, N. Nutkumhang, M. P. Mammen and R. G. Jarman, "Dengue Virus Detection Using Whole Blood for Reverse Transcriptase PCR and Virus Isolation", J Clin Microbiol, 45 (8), 2480-2485 (2007).
109.D. W. Leung, G. Cachianes, W. J. Kuang, D. V. Goeddel and N. Ferrara, "Vascular Endothelial Growth-Factor Is a Secreted Angiogenic Mitogen", Science, 246 (4935), 1306-1309 (1989).
110.S. M. Wang, L. Ge, X. R. Song, J. H. Yu, S. G. Ge, J. D. Huang and F. Zeng, "Paper-based chemiluminescence ELISA: Lab-on-paper based on chitosan modified paper device and wax-screen-printing", Biosens Bioelectron, 31 (1), 212-218 (2012).
111.S. W. Wang, L. Ge, Y. Zhang, X. R. Song, N. Q. Li, S. G. Ge and J. H. Yu, "Battery-triggered microfluidic paper-based multiplex electrochemiluminescence immunodevice based on potential-resolution strategy", Lab Chip, 12 (21), 4489-4498 (2012).
112.P. Rattanarat, W. Dungchai, W. Siangproh, O. Chailapakul and C. S. Henry, "Sodium dodecyl sulfate-modified electrochemical paper-based analytical device for determination of dopamine levels in biological samples", Anal Chim Acta, 744, 1-7 (2012).
113.C. G. Shi, X. Shan, Z. Q. Pan, J. J. Xu, C. Lu, N. Bao and H. Y. Gu, "Quantum Dot (QD)-Modified Carbon Tape Electrodes for Reproducible Electrochemiluminescence (ECL) Emission on a Paper-Based Platform", Analytical Chemistry, 84 (6), 3033-3038 (2012).
114.S. A. Klasner, A. K. Price, K. W. Hoeman, R. S. Wilson, K. J. Bell and C. T. Culbertson, "Paper-based microfluidic devices for analysis of clinically relevant analytes present in urine and saliva", Anal Bioanal Chem, 397 (5), 1821-1829 (2010).
115.A. W. Martinez, S. T. Phillips, E. Carrilho, S. W. Thomas, H. Sindi and G. M. Whitesides, "Simple telemedicine for developing regions: Camera phones and paper-based microfluidic devices for real-time, off-site diagnosis", Analytical Chemistry, 80 (10), 3699-3707 (2008).
116.T. M. Blicharz, D. M. Rissin, M. Bowden, R. B. Hayman, C. DiCesare, J. S. Bhatia, N. Grand-Pierre, W. L. Siqueira, E. J. Helmerhorst, J. Loscalzo, F. G. Oppenheim and D. R. Walt, "Use of colorimetric test strips for monitoring the effect of hemodialysis on salivary nitrite and uric acid in patients with end-stage renal disease: A proof of principle", Clin Chem, 54 (9), 1473-1480 (2008).
117.A. W. Martinez, S. T. Phillips, G. M. Whitesides and E. Carrilho, "Diagnostics for the Developing World: Microfluidic Paper-Based Analytical Devices", Analytical Chemistry, 82 (1), 3-10 (2010).
118.M. Schwanninger, J. C. Rodrigues, H. Pereira and B. Hinterstoisser, "Effects of short-time vibratory ball milling on the shape of FT-IR spectra of wood and cellulose", Vib Spectrosc, 36 (1), 23-40 (2004).
119.P. Favia, G. Cicala, A. Milella, F. Palumbo, R. Rossini and R. d''Agostino, "Deposition of super-hydrophobic fluorocarbon coatings in modulated RF glow discharges", Surface &; Coatings Technology, 169, 609-612 (2003).
120.I. T. Martin, G. S. Malkov, C. I. Butoi and E. R. Fisher, "Comparison of pulsed and downstream deposition of fluorocarbon materials from C3F8 and c-C4F8 plasmas", Journal of Vacuum Science &; Technology A, 22 (2), 227-235 (2004).
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