基於光子晶體(Photonic Crystal, PC)和分子拓印聚合物(Molecularly Imprinted Polymer, MIP)的組合，本研究開發出一種可於自來水來中快速、無須標記針對雙酚A (Bisphenol A, BPA)檢測的分子拓印聚合物智能感測器。分子拓印光子晶體感測器(Molecularly Imprinted Photonic Crystal, MIPC)由分子拓印水凝膠膜和單分散二氧化矽(SiO2)膠體粒子自組裝方式所得的光子晶體模板所構成，分子拓印水凝膠膜由功能性單體甲基丙烯酸(Methacrylic acid, MAA)、交聯劑乙二醇二甲基丙烯酸酯(Ethylene Glycol Dimethacrylate, EGDMA)和模板分子BPA在BPA/MAA/EGDMA摩爾比=1:5:2.5所構成。爾後，去除SiO2膠體模板和模板分子BPA後，所得的MIPC具有三維結構、高度有序且相互連接的大孔陣列組成的薄水凝膠層，通過形狀和官能基位置與目標分子互補的拓印孔洞於水溶液中吸附後，基於MIPC結構響應其與目標分子的再結合而發生的晶格變化，可藉由布拉格衍射峰紅移來檢測MIPC對水樣中BPA分子的響應，所製備的MIPC可於4 分鐘內響應BPA濃度，動態濃度檢測範圍可達0.2-100 mg/L，最低偵測極限為0.13 mg/L，相較於BPF與phenol，對BPA的檢測選擇性可達4倍，使用後的MIPC可經甲醇/醋酸(9:1, V/V)萃洗BPA分子後回復感測能力，於10次反覆吸-脫附程序後，訊號回復率可達99.5 %，標準差為0.996，並通過鹽析作用提高本MIPC的靈敏度於實際水樣中的感測範圍可達0.03-0.6 mg/L，且最低偵測極限提升至6×10-3 mg/L。此MIPC可用於視覺推估水樣中BPA的濃度，且無需使用標記技術和貴重儀器即可實現於實際水樣中針對BPA分子直接和選擇性的檢測，使本MIPC在現場篩選和視覺檢測實際水樣中的檢測具有莫大的潛力。

Based on the combination of a photonic crystal (PC) and molecular imprinting polymer (MIP), we have developed a label-free molecular (molecularly) imprinted sensor for bisphenol A (BPA) detection with high sensitivity and fast response. The molecularly imprinted photonic crystal (MIPC) sensor was composed of a molecularly imprinted hydrogel film and a photonic crystal template which was constructed by self-assembled SiO2 colloids. The molecular imprinted hydrogel film was composed of functional monomer methacrylic acid (MAA), cross-linker ethylene glycol dimethacrylate (EGDMA), and template BPA at the molar ratio of BPA/MAA/EDGMA of 1:5:2.5. After removing the colloidal crystal template and the imprinted BPA molecules, the resulting imprinted inverse opal photonic crystal sensor had a three-dimensional structure, highly ordered, and interconnected macroporous structure. With BPA binding by the imprinted cavities within the hydrogel, expanding the lattice of the MIPC red shifted the diffraction light. The MIPC was able to respond to BPA within 4 minutes with a wide dynamic range (0.2-100 mg/L) and a low detection limit (0.13 mg/L). In addition, it exhibited 4 times higher wavelength shift with respective to BPF and phenol. The used sensor can be recovered by washing with methanol/acetic acid (9:1, V/V) and the sensing ability after 10 times of adsorption-desorption procedures still maintained 99.5% with a small variation of 0.996. With salting-out effect, the detectable BPA concentration in the tap water was remarkably decreased to 0.03 mg/L with a detection limit of 6×10-3 mg/L. This sensor can be used to visually estimate the concentration of BPA in the water sample without the use of labeling technology and expensive instruments and is promising to be applied for on-site screening.

主目錄
摘要.....I
Abstract......II
主目錄.....IV
表目錄.....V
圖目錄.....VI
第一章 前言...VI
1.1 研究背景與動機...1
1.2 研究目的...4
第二章 文獻回顧...5
2.1 分子拓印材料...5
2.2 光子晶體 (Photonic crystal, PC)...11
2.3 拓印光子晶體感測器(Impinted Photonic Crystal, IPC)...21
2.4 光子晶體感測器於實際樣品中應用...26
第三章 研究方法...31
3.1實驗材料...33
3.2分子拓印光子晶體感測器...34
3.3感測能力試驗...36
3.4儀器分析...39
第四章 結果與討論...41
4.1 分子拓印光子晶體感測器...41
4.2 分子拓印高分子聚合物...47
4.3 去離子水中感測能力試驗...51
4.4 自來水中的BPA分析...57
第五章 結論與建議...64
5.1 結論...64
5.2 未來建議...65
參考文獻...66
附錄...72

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