以溶膠－凝膠程序製備磺胺二甲嘧啶無機分子拓印高分子

本研究以磺胺二甲嘧啶 (Sulfamethazine, SMZ) 為模板分子，四甲氧基矽烷(Tetramethoxysilane, TMOS) 和一甲基三甲氧基矽烷 (Methyltrimethoxysilane, MTMOS) 為單體，經溶膠-凝膠程序製備無機分子拓印高分子 (inorganic molecularly imprinted polymer, IMIP) 。所討論的變數為 (1) 反應系統的R值 (H2O/Si molar ratio) (2) 競爭吸附實驗中標準溶液pH值 (3) 鍛燒溫度 (4) TMOS之比例 (5) HCl添加量 (6) 系統反應溫度，最後再以高效能液相層析儀 (high performance liquid chromatographic method, HPLC) 測量SMZ與相似物磺胺甲噁唑 (Sulfamethoxazole, SMO) 濃度進而算出吸附量與選擇率。結果顯示當競爭吸附實驗中標準溶液pH值接近模板分子的pKa2值時(pH=7.4) 可有效提高選擇率。其中IMIP之SMZ吸附量會隨著R值和第二階段鍛燒溫度上升而增加。TMOS之比例會影響無機網目的交聯密度和柔軟性，最後再適當改變HCl添加量和反應溫度。結果顯示當標準溶液pH值為7.4， R值為10，第二階段鍛燒溫度為375℃，TMOS比例為1， HCl添加量為750 μl和反應溫度為80℃下，可獲得最高的選擇率 (α=21.8) 且辨識效果比無拓印高分子 (non-imprinted polymer, NIP) 更佳。

關鍵字

無機分子拓印高分子；溶膠-凝膠程序；磺胺二甲嘧啶(SMZ) ；選擇率

並列摘要

Inorganic molecularly imprinted polymer (IMIP) based on tetramethoxysilane (TMOS) and methyltrimethoxysilane (MTMOS) by sol-gel process has been developed. The conditions of preparation, the ratio of water to monomers (R), pH value of competition solution, calcination temperature, the ratio of TMOS to monomers (TMOS ratio), amount of hydrochloric acid and the reaction temperature were investigated. The competition experiment of the IMIP for template (sulfamethazine, SMZ) and analogue(sulfamethoxazole, SMO) were analyzed by High-Performance Liquid Chromatography (HPLC). The results showed that the higher selectivity of IMIP was obtained when pH value of competition solution was set to the pKa2 of SMZ. In addition, the adsorption of SMZ was increased with increase of the R value and the 2nd step calcination temperature. The crosslink and flexible of network were affected by TMOS ratio. Finally, amount of hydrochloric acid and the reaction temperature were also adjusted appropriately. The results showed that the best selectivity (α=21.8) of IMIP were obtained with R=10, the pH value of competition solution = 7.4, TMOS ratio = 1, amount of hydrochloric acid was 750 μl, the reaction temperature = 80℃ and the 2nd step calcination temperature =375°C. The IMIP (AdSMZ=2.18 μmol/g, α=21.8) was obtained the more efficiency than non-imprinted polymer (AdSMZ=1.62 μmol/g, α=6.23).

並列關鍵字

sulfamethazine ； selectivity ； sol-gel process ； Inorganic molecularly imprinted polymer

參考文獻

1. Fischer, E.,“Einfluss der configuration auf die wirkung derenzyme”, Chem. Ber., Vol.27, pp. 2985-1993, 1894

2. Ramstrom, O., L.I. Andersson, and K. Mosbach,“RECOGNITION SITES INCORPORATING BOTH PYRIDINYL AND CARBOXY FUNCTIONALITIES PREPARED BY MOLECULAR IMPRINTING”, Journal of Organic Chemistry, Vol.58, pp. 7562-7564, 1993

3. L.Pauling,“A Theory of the Structure and Process of Formation of Antibodies”, Journal of the American Chemical Society Vol.62, pp. 2643-2657, 1940

4. Ye, L., I. Surugiu, and K. Haupt,“Scintillation proximity assay using molecularly imprinted microspheres”, Analytical Chemistry, Vol.74, pp. 959-964, 2002

5. Marx, S., et al.,“Parathion sensor based on molecularly imprinted sol-gel films”, Analytical Chemistry, Vol.76, pp. 120-126, 2004

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以溶膠－凝膠程序製備磺胺二甲嘧啶無機分子拓印高分子

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