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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彭均莉(Chun-li Peng) 查詢紙本館藏

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化學工程與材料工程學系

論文名稱

以溶膠－凝膠程序製備磺胺二甲嘧啶無機分子拓印高分子
(Preparation of inorganic molecularly imprinted polymers based on Sulfamethazine by sol–gel process)

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摘要(中)

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。

摘要(英)

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).

關鍵字(中)

★ 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

關鍵字(英)

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

論文目次

中文摘要 ………………………………………………………… i
英文摘要 ………………………………………………………… ii
誌謝 ………………………………………………………… iii
目錄 ………………………………………………………… iv
圖索引 ………………………………………………………… vi
表索引 ………………………………………………………… viii
第一章前言…………………………………………………… 1
1-1 分子拓印高分子發展及應用………………………… 1
1-2 分子拓印高分子技術與原理………………………… 2
1-3 溶膠－凝膠程序……………………………………… 4
1-3-1 系統之pH值對溶膠－凝膠程序的影響……………… 4
1-3-2 含水量對溶膠－凝膠程序的影響…………………… 5
1-3-3 矽偶合劑添加對溶膠－凝膠程序的影響…………… 5
1-4 文獻回顧……………………………………………… 7
1-5 模板分子SMZ之介紹………………………………… 8
1-6 研究目的……………………………………………… 9
第二章實驗…………………………………………………… 10
2-1 實驗藥品……………………………………………… 10
2-2 實驗儀器……………………………………………… 12
2-3 無機分子拓印高分子之製備………………………… 13
2-4 無機分子拓印高分子之物性測試…………………… 15
2-4-1 競爭吸附實驗………………………………………… 15
2-4-2 氮氣吸附孔隙儀分析………………………………… 15
2-4-3 紅外線光譜分析……………………………………… 15
2-4-4 熱重分析儀分析……………………………………… 15
第三章結果與討論…………………………………………… 16
3-1 R值對於無機分子拓印高分子的影響………………… 16
3-2 標準溶液pH值對於無機分子拓印高分子的影響…… 23
3-3 鍛燒溫度對無機分子拓印高分子的影響…………… 29
3-4 四甲氧基矽烷比例對無機分子拓印高分子的影響… 36
3-5 HCl添加量對於製備無機分子拓印高分子之影響…… 43
3-6 系統反應溫度於製備無機分子拓印高分子響……… 50
3-7 比較有無添加模版分子SMZ之無機分子拓印高分子… 53
第四章結論…………………………………………………… 55
參考文獻……………………………………………… 57

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指導教授

陳暉(Hui Chen)

審核日期

2008-6-20

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