本研究提出利用低成本的聚酯纖維線，製作第一個整合電泳分離電化學檢測，與電噴灑游離質譜偵測之微流體晶片，並將其應用於生醫與食品樣本之分析。本研究選用200 µm的市售縫紉用聚酯纖維線，做為樣本傳輸與偵測的微流道，其成本非常低廉，且取得容易，適合發展可攜、拋棄式檢測裝置。傳統微流體晶片多使用十字型或雙T字型的樣本注入設計，本研究打破傳統的概念，僅利用一條聚酯纖維線完成樣本的注入、分離與檢測。此創新的設計亦帶來許多好處，例如晶片製程與樣本注入步驟簡單化，樣本注入位置的自由度提高等等。此外，本研究發明一項線上樣本聚焦技術，其不需使用任何能源設備與複雜的操作，只透過線材本身的毛細作用力，即可完成樣本塊長度縮小與樣本濃縮。經過影像與檢測訊號分析結果得知，原本在線上完全展開的樣本塊，經過樣本聚焦後長度被縮短成原本的38%，再從電化學安培偵測結果得知，聚焦後樣本的氧化還原電流響應，比未經聚焦的樣本提升了2.7倍，其理論板數值亦提高了2.8倍。本研究利用簡單的夾具結構，固定住聚酯纖維線的其中一端，形成噴嘴的結構，再利用高壓電場於此前端產生電噴灑游離。此設計不需要複雜的製程方法或結合專門的噴嘴，也不需要使用溶液注射泵浦與輔助鞘流氣體，即可產生穩定的電噴灑與良好的游離效果，在電場為6.5×105 V/m的條件下，聚酯纖維線電噴灑游離能維持109 ions/cm3的高總離子濃度長達30 min。質譜檢測結果顯示，本系統不管是針對一般極性樣本、弱極性樣本、或複雜組成的食品樣本，偵測訊號之信噪比皆能達到10以上，有很好的成分分析能力。最後，本研究利用線微流體系統，將電泳電化學檢測技術整合於電噴灑游離質譜法，發展低成本，但高效能且檢測對象範圍廣泛的微流體晶片。本研究透過檢測生醫樣本多巴胺與抗壞血酸，以及組成物質複雜之舒跑運動飲料，證實將電泳電化學與電噴灑質譜法結合，不但能雙重檢查檢測結果，更能互補兩種方法的限制，於生醫或食品領域之應用有極大的潛力。

This research presents the first microfluidic chip for integration of capillary electrophoresis electrochemical (CE-EC) detection and electrospray ionization (ESI). It can be used for rapid bio and food sample analysis. Polyester thread of 200 µm in diameter is used as the liquid route such that delicate channel fabrication process can be excluded. The entire detection process of this system can be done by only a straight polyester thread channel, which break the conventional concept of sample manipulation. This new design also bring us some benefits, such as liquid sample can be directly applied at arbitrary site of the thread for electrophoresis separation. In order to improve the efficiency of single thread based CE separation, two buffer drops are applied at neighboring side of the sample plug to shorten it, which is called in-line sample pinch focus process. Image results shows that the length of sample plug can be reduced to about 38% of its original after the focus process. In addition, the current response of EC detection shows 2.7 times enhancement, and the theoretical plate number also increase 2.8 times. A simple fixture structure is designed to hold the thread, and the tail end of thread is then applied a high voltage for ESI. The thread-based ESI can easy be stabilized for more than 30 min with a high ion intensity of 109 ions/cm3. The ingredients of commercial eye drops and energy drink-Red Bull are detected with high signal to noise ratio of more than 10. Finally, the combination of CE-EC detection and ESI is achieved by the developed single thread microfluidic. Bio samples of dopamine and ascorbic acid, and food sample of Supau are both successfully be detected by these two methods. The combination of two detection methods can let them complement each other's shortage, which shows great potential for bio and food applications.

論文審定書 i
論文授權書 ii
致謝 iii
中文摘要 iv
Abstract v
目錄 vi
圖目錄 ix
表目錄 xi
符號表 xii
簡寫表 xiii
第一章 緒論 1
1.1 研究背景 1
1.2 微流體晶片系統簡介 2
1.2.1 矽與玻璃材料微流體晶片 2
1.2.2 高分子材料微流體晶片 4
1.2.3 紙微流體晶片 5
1.2.4 線微流體晶片 7
1.3 毛細管電泳分離法 11
1.3.1 毛細管電泳簡介 11
1.3.2 毛細管電泳晶片常用材料與其EOF比較 12
1.3.3 毛細管電泳效能分析與影響效能的因素 14
1.4 電噴灑游離法 16
1.4.1 電噴灑游離法之發展 16
1.4.2 電泳電噴灑晶片常見之設計 17
1.4.3 紙電噴灑晶片 19
1.4.4 燭芯電噴灑法 21
1.5 研究動機與目的 23
1.6 論文架構 24
第二章 實驗原理與材料特性 25
2.1 聚酯纖維線特性與電漿表面改質 25
2.2 線上樣本聚焦原理 27
2.3 毛細管電泳分離法原理 28
2.4 電噴灑游離質譜偵測法原理 31
2.4.1 一般電噴灑游離 31
2.4.2 電暈放電輔助電噴灑游離機制 32
第三章 實驗設計與架構 34
3.1 線微流體晶片設計 34
3.1.1 直線型流道設計 34
3.1.2 線微流體電泳電噴灑晶片 35
3.2 壓克力基板製程簡介 36
3.3 實驗設計與檢測目標 38
3.4 實驗操作流程 39
3.5 系統架設與實驗設備 41
3.6 實驗溶液配製 44
第四章 實驗結果與討論 46
4.1 線上樣本聚焦效能分析 46
4.1.1 樣本聚焦效能-影像分析 46
4.1.2 樣本聚焦效能-訊號分析 47
4.1.3 樣本聚焦效能比較表 48
4.2 聚酯纖維線電噴灑效能分析 50
4.2.1 電噴灑游離影像分析 50
4.2.2 穩定電噴灑條件測試 53
4.2.3 線電噴灑長時間穩定度測試 54
4.3 聚酯纖維線電噴灑樣本檢測結果 55
4.3.1 一般極性單一樣本檢測 55
4.3.2 複雜組成之食品樣本檢測 57
4.3.3 弱極性樣本檢測 58
4.4 電泳電化學結合電噴灑質譜法檢測結果 60
第五章 結論與未來展望 64
5.1 結論 64
5.2 未來展望 66
參考文獻 67
自述 75

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