傳統食品安全檢測採用HPLC/MS等技術，此類儀器設備與耗材皆昂貴，而且需要專業訓練操作員，目前大多將肉品送到特定實驗中心進行檢驗，無法快速現場檢測。過去本實驗室已發展出可圖案化電沉積壓電高分子製程來製作聲波微收發器，然而良率隨著製程人員經驗而不同。本論文首先在此基礎上進一步改善製程，提升壓電薄膜與金電極接合力與製程良率;接著以為實現全整合生醫感測器之目標，將分子拓印高分子直接電沉積於聲波接收器上，使得聲波接收器提升專一性之吸附能力，實現以生醫感測器來完成食品肉汁殘留藥物快速檢測。
本研究為提升製程良率，以烯丙基硫醇(Allyl Mercaptan)在來壓電薄膜與金電極間形成金-硫(Au-S)共價鍵，加強材料間接合力，使得薄膜覆蓋面積達90 % 以上的製程良率，從原本的10 % 以下提升至大於90 %，且訊號調控前的壓電薄膜訊號也比原先提升37.5% (10 kHz)，所配置之添加烯丙基硫醇的P(VDF-TrFE)的DMSO溶液，具有約五個月的時效性。本論文以Doxycycline作為檢測目標，微流體晶片設計上，分為單階段檢測晶片設計與兩階段檢測晶片設計，單階段設計僅有1次流體操作與1次專一辨識分離;而兩階段設計則有2次流體操作與2次專一辨識分離。單階段微流體直接對肉汁進行檢測下，檢測區間在0 ppb至300 ppb，靈敏度為0.5 mV/ppb，附錄G所補充的實驗中在0.0008 ppb 下仍然有53.9 dB的高訊雜比(SNR)；FAPAS豬肉肉汁檢測方面，以兩階段檢測晶片設計來測試，結果為163.6 ppb，與最終答案166.6 ppb 相差1.4 %，全球63間參與檢驗測試實驗室中準確度排行第三。
本研究所提出之高靈敏聲波壓電生醫感測器，全整合專一性辨識於微感測器，具備有簡易操作、高準確性與低檢測極限以及快速檢測系統整合的特點。

Traditional food safety testing uses technologies such as HPLC/MS. These instruments and consumables are expensive, and professional training operators are required. At present, most of the meat is sent to a specific experimental center for inspection, and it is not possible to quickly detect it on site. In the previous work, the laboratory has developed a patterned electrodeposition piezoelectric polymer process to make acoustic micro-transceivers, but the yield varies with the experience of the process personnel. On the basis of previous works of laboratory, this paper further improves the process by to create strong bonding force of the piezoelectric film and the gold electrode. Then, in order to achieve the goal of fully integrated biomedical sensor, the molecularly imprinted polymer is directly electro polymerized on the acoustic biosensor receiver. On the device, the molecularly imprinted polymer enhances the sensitivity and specificity, and realizes the rapid detection of the residual drug of the food.
In order to improve the yield of the process, Allyl Mercaptan is used to form a gold-sulfur (Au-S) covalent bond between the piezoelectric film and the gold electrode to strengthen the bonding force between the materials, so that the film coverage area is up to More than 90 % of the process yield increased from less than 10 % to more than 90 %, and the piezoelectric film signal before signal conditioning was also increased by 37.5% (10 kHz), with the addition of Allyl Mercaptan. A solution of P(VDF-TrFE) in DMSO has period of validity of about five months. In this paper, Doxycycline is used as the detection target. The microfluidic chip design is divided into single-stage detection chip design and two-stage detection chip design. The single-stage design has only one fluid operation and one specific identification separation. The two-stage design has Two fluid operations were separated from two specific identifications. The single-stage microfluid directly measures the meat sample fluid with a detection range of 0 ppb to 300 ppb and a sensitivity of 0.5 mV/ppb. The experiment supplemented by Appendix G still has a high signal-to-noise ratio (SNR) of 53.9 dB at 0.0008 ppb. The FAPAS meat sample test was tested with a two-stage test wafer design with a result of 163.6 ppb, a difference of 1.4% from the final answer of 166.6 ppb, and the third highest accuracy among 63 participating test laboratories worldwide.
The high-sensitivity acoustic piezoelectric biosensor proposed by the research institute is fully integrated and uniquely recognized in the micro-sensor, and has the characteristics of simple operation, high accuracy, low detection limit and rapid detection system integration.

目錄
摘要 1
Abstract 2
誌謝 4
目錄 5
圖目錄 8
表目錄 13
第一章 緒論 14
1.1 食品安全檢測 14
1.2傳統檢測方式 16
1.2.1 質譜儀 17
1.2.2 液相層析技術 18
1.2.3 酵素免疫分析法 23
1.3 低濃度生醫感測器 25
1.3.1 電化學感測器 26
1.3.2 光學感測器 28
1.3.3 螢光感測器 30
1.3.4 壓電石英感測器 34
1.3.5 表面聲波感測器 38
1.3.6 壓電式聲波微傳感器 39
1.4 分子辨識 40
1.5 研究動機 42
1.6 研究目的 43
1.7 論文研究架構 44
第二章 聲波感測器之結構原理與製程改善 46
2.1 壓電聲波感測器結構 46
2.2 壓電感測薄膜特性與感測原理 48
2.3壓電高分子材料與製程 52
2.3.1 壓電高分子材料 52
2.3.2 壓電高分子製程 54
2.3.3 電沉積薄膜均勻性 59
2.5 壓電薄膜製程改善 61
2.5.1 薄膜覆蓋率計算 61
2.5.2 電壓與製程良率關係探討 62
2.5.3 電極表面清潔與良率關係探討 65
2.5.4添加硫醇基提升薄膜製程良率 66
2.5.5 壓電薄膜電沉積藥物時效性 70
2.5.6 基材表面改質微液滴成型 73
2.6 硫醇基壓電薄膜製程性能量測 74
2.6.1 訊號強度 74
2.6.2 預振調控響應準位試驗 76
2.6.3 輸入電壓調整裝置輸出訊號 78
第三章 分子拓印導電高分子壓電聲波感測器開發 80
3.1 分子拓印導電高分子技術 80
3.1.1 分子拓印高分子技術 80
3.1.2 導電高分子技術 84
3.1.3 導電高分子結合分子拓印 85
3.2 壓電高分子薄膜結合分子拓印技術開發規劃 88
3.3 壓電高分子薄膜混和拓印分子技術開發 90
3.3.1 壓電高分子溶液混和待測藥物電沉積實驗 91
3.3.2 電聚合拓印分子定電壓動態實驗 93
3.3.3 電聚合拓印分子定電流動態實驗 95
3.3.4 分子拓印高分子甲醇沖洗耐受實驗 96
3.3.5 傅立葉轉換紅外光譜(FTIR)拓印分子檢測實驗 97
3.3.6 壓電薄膜表面電子顯微鏡(SEM)觀測 101
3.4 壓電聲波生醫感測器性能量測 103
3.4.1 分子拓印高分子修飾對於訊號靈敏度提升試驗 103
3.4.2 壓電聲波生醫感測器專一性量測 104
3.4.3 壓電聲波生醫感測器反覆沖洗動態量測 105
3.4.4 準位調整後肉汁試驗 106
3.4.5 壓電聲波生醫感測器穩定所需時間量測 107
第四章 壓電聲波生醫感測器應用於食品快篩檢測 108
4.1 生醫感測器於食品安全之應用 108
4.2 動物用藥殘留檢測項目 110
4.3 應用於食安藥物殘留快速檢測碟片 113
4.4 壓電聲波感測器肉汁量測 118
4.5 結論 121
第五章 總結與研究成果 122
5.1 總結 122
5.2 研究成果 123
5.3 研究創新 125
5.4 學術貢獻 129
5.5 未來研究建議 134
附錄 135
附錄A：聲波量測儀器規格 135
附錄B：Labview訊號處理 138
附錄C：化學藥品名稱 140
附錄D：製程詳細步驟 141
附錄E：電沉積製程治具 142
附錄F：檢測用肉汁處理及取得方式 143
附錄G：最低濃度檢測 144
附錄H：英國分析實驗室能力驗證 ( FAPAS, Food Analysis Performance Assessment Scheme ) 145
附錄F : 頻率響應補充實驗 149
參考資料 150
作者簡介 158
著作發表 160

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