利用超臨界二氧化碳合成甲基丙烯酸與阿魏酸共聚物之抗氧化性高分子材料

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题名:	利用超臨界二氧化碳合成甲基丙烯酸與阿魏酸共聚物之抗氧化性高分子材料
作者:	曾梨子
贡献者:	化工系
关键词:	超臨界聚合反應高分子型抗氧化劑阿魏酸
日期:	2011~2012
上传时间:	2012-02-24 09:41:07 (UTC+8)
摘要:	在目前的高污染的環境當中，如何減少自由基對於人體或食物的危害，成為一大重要課題。而抗氧化劑能與自由基起作用，穩定自由基，避免自由基與其他分子反應，且高分子抗氧化劑具有較高的穩定性及緩慢的分解速率，因此將抗氧化劑固定於高分子鏈上可降低抗氧化劑的擴散損失。近年來，許多研究利用超臨界流體特殊的物理性質，當作材料合成、加工的媒介，特別是用於醫藥、食品方面之材料合成，其中，高分子型抗氧化劑的合成最為常見。有鑑於此，本計畫也針對將抗氧化劑以共聚合反應連接到高分子材料主體，以期能得到高分子抗氧化劑共聚物之材料，對抗氧化劑改質方法做深入的研究。為了避免溶劑的殘留及綠色環境的策略，本研究將探討利用高壓設備，以超臨界二氧化碳(Supercritical carbon dioxide, SCCO2)為溶媒，使用超臨界技術進行合成製備高分子型抗氧化劑材料，其中，偶氮二異丁腈(AIBN)當作起始劑，甲基丙烯酸(MAA)為單體，小分子抗氧化劑阿魏酸(FA)為共聚單體，交聯劑二甲基丙烯酸乙二醇酯(EGDMA)，進行自由基加成聚合反應，製備兩種結構的高分子型抗氧化劑，分別為線型共聚高分子PMAA-FA與網狀結構高分子PMAA-FA-EGDMA，此兩種型式的高分子抗氧化劑材料，主要可應用於藥物或醫療方面。第一年的研究，將已建立的超臨界流体反應設備，製備線型共聚高分子PMAA-FA，並利用材料分析以傅立葉轉換紅外線光譜(FTIR)及紫外可見光光譜(UV-Vis spectrometer) 分析MAA與FA含量分析，核磁共振氫譜(1H NMR)鑑定共聚物之化學結構；熱重分析(TGA)測量材料熱裂解溫度(Td)；抗氧化性質分析以DPPH法測試得氧化抑制百分比；電子顯微鏡(SEM)觀察表面形貌，並進一步深入探討反應參數如起始劑濃度及反應物單體濃度等反應因素對產物物性的影響。本研究第二年，製備網狀結構高分子PMAA-FA-EGDMA，除尋求反應槽SCCO2的壓力、溫度及時間等最適操作條件，並將實驗數據進行歸納分析，將可整理出超臨界共聚合反應的研究參數關聯性與最適化關鍵因素，評估實際應用的可能性並作為相關研究的參考，此兩種結構的高分子型抗氧化劑可廣泛應用於醫藥領域。 In the present highly polluted environment, the diminishing of the contamination of free radical in human bodies and food has become an important topic to many researchers. Antioxidant can react with free radical to avoid the reaction of free radical with other compounds. And Antioxidant in a polymer form is more stable and can slow down the releasing rate. Copolymerization of antioxidant with a polymer can also reduce the diffusing lost of antioxidant. In this project, the reaction of an antioxidant with monomer to form a copolymer product using supercritical fluid technology is studied. The copolymerization reaction of antioxidant with monomers has traditionally been synthesized using organic solvents. For the sake of avoided solvent residue and environmental protection, those traditional methods can be replaced by other green processes. The strategy that using supercritical carbon dioxide as green solvent, methacrylic acid(MAA) as monomer, antioxidant ferulic acid(FA) as comonomer and ethylene glycol dimethacrylate (EGDMA) as crosslinker is suggested, and the addition polymerization will proceed with initiator AIBN. In the first year of this study, the copolymerization reaction linear copolymer PMAA-FA is investigated. The chemical properties of the result product can be identified by FTIR, UV-Vis spectrums and 1H NMR, and the degrading temperature of polymeric antioxidant is studied by TGA. Antioxidant ability is measured by DPPH assay. And SEM images will show the size and morphology of products. Moreover the effects of concentrations of initiator, antioxidant and monomer reactants will also be studied. In the second year, the network form of polymeric antioxidant PMAA-FA-EGDMA is synthesis. We will also investigate the effects of reaction factors such as the temperature, pressure and reaction time period in SCCO2. The operation conditions and the reaction parameters will be optimized through this investigation. The results for optimal operation conditions are expected that are valuable to future industrial applications. The two forms of polymeric antioxidants could be useful in pharmaceutical and medical applications.
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