高度纏結的雙離子水凝膠

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莊英傑(Ying-Chieh Chuang) 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

高度纏結的雙離子水凝膠
(Highly entangled zwitterionic hydrogels)

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至系統瀏覽論文 (2029-7-1以後開放)

摘要(中)

水凝膠是一種透過交聯而形成的親水性聚合物三維網絡，具有高度的保水能力，由於其具有高生物相容性、可調節的機械性能，被廣泛應用於生醫工程領域。然而，大部分的水凝膠無法有效防止蛋白質、細菌沾黏導致嚴重的感染與異物反應。更重要的是，水凝膠的應用很大程度受限於其機械性質的強弱與特性。為了實現抗非特異性吸附，人們開始了對各種材料的研究。雙離子材料因其優異的抗非特異性吸附能力而被視為生醫材料中非常具有潛力的材料之一。然而，其應用受限於較弱的機械強度，因此如何改善機械性質對於雙離子材料是非常重要的。在此研究中，我們以高密度的物理纏結(Entanglement)形成的物理交聯取代傳統使用交聯劑形成共價鍵的化學交聯，透過調整水凝膠聚合物網絡中的化學交聯及物理交聯實現能量逸散，使該水凝膠具有高韌性、可拉伸性、低滯後性及潤滑之特性。為了比較分子間氫鍵與網絡均勻度對高度纏結效應造成的影響，比較了四種結構之雙離子分子: Sulfobetaine methacrylate（SBMA）、Sulfobetaine acrylate（SBA）、Sulfobetaine acrylamide（SBAA）和Sulfobetaine methacrylamide（SBMAA），透過核磁共振光譜儀(NMR)對SBA、SBMA、SBAA和SBMAA分子結構進行鑑定並進行準一級聚合反應測試(Pseudo-first-order polymerization kinetics)測試各分子結構之反應速率。並選用N,N’-Methylenebisacrylamide (MBAA)和N,N′-Methylenebismethacrylamide (MBMA)作為交聯劑，成功聚合了不同均勻度的水凝膠以動態光散射儀(Dynamic Light Scattering, DLS)分析其均勻程度，並使用萬能拉力機分析水凝膠機械性質以及其與網絡均勻度之關係。使用萬能拉力機檢測水凝膠機械性質以及滯後試驗。使用傅立葉轉換紅外線光譜儀(Fourier-Transform Infrared Spectroscopy, FTIR)、原子力顯微鏡(Atomic Force Microscope, AFM) 、客製化萬能拉力機與動態機械分析儀(Dynamic Mechanical Analyzer, DMA)分析了水凝膠結構內分子間氫鍵強度、表面吸附能與摩擦係數與黏彈特性。並透過細菌及蛋白質測試探討了高度纏結效應對抗非特異性吸附效果之影響。本論文透過比較四種分子結構探討了不同變因對高度纏結效應之影響，藉此探討如何設計出符合實際應用需求之機械性質特性之雙離子水凝膠。

摘要(英)

Hydrogels are three-dimensional networks of hydrophilic polymers formed through crosslinking. Owing to their high water retention capacity, high biocompatibility and controllable mechanical properties, it has extensive applications in the field of biomedical engineering. However, most of hydrogels fail to effectively prevent protein and bacterial adhesion, leading to severe infections and foreign body reactions. More importantly, the application of hydrogels is constrained by their mechanical properties, including strength and characteristics. To achieve anti-nonspecific adsorption, researchers have begun to investigate various materials. Zwitterionic materials are considered very promising materials in biomedical materials due to their excellent anti-nonspecific adsorption. However, its application is limited by weak mechanical properties. Therefore, improving mechanical properties is crucial for zwitterionic materials. In this study, we present a novel approach to overcome this limitation by preparing highly entangled zwitterionic hydrogels, which exhibit high toughness, stretchability and low hysteresis by adjusting the polymerization conditions to optimize the balance between physical and chemical cross-links through entanglements and covalent bonds, respectively to achieve energy dissipation. To compare the impact of intermolecular hydrogen bonding and network homogeneity on the highly entangled effect, four types of zwitterionic molecules were compared: Sulfobetaine methacrylate (SBMA), Sulfobetaine acrylate (SBA), Sulfobetaine acrylamide (SBAA), and Sulfobetaine methacrylamide (SBMAA). Nuclear magnetic resonance spectroscopy (NMR) was employed to identify the molecular structures of SBA, SBMA, SBAA, and SBMAA, followed by pseudo-first-order polymerization kinetics tests to measure the reaction rates of each molecular structure. We used N,N’-Methylenebisacrylamide (MBAA) and N,N′-Methylenebismethacrylamide (MBMA) as crosslinkers to successfully synthesize hydrogels with varying degrees of homogeneity. The homogeneity of hydrogels were analyzed by dynamic light scattering (DLS), while their mechanical properties were analyzed by the universal testing machine to conform the relationship between mechanical properties and network homogeneity. Mechanical properties and hysteresis were analyzed by the universal testing machine. Fourier transform infrared spectroscopy (FTIR), atomic force microscopy (AFM), customized universal testing machines, and dynamic mechanical analysis (DMA) were employed to analyze the strength of intermolecular hydrogen bonds, surface adsorption energy, friction coefficient, viscosity and elasticity characteristic of the hydrogels. Furthermore, bacterial and protein tests were conducted to investigate the impact of the highly entangled effect on anti-nonspecific adsorption. This study compares the effects of different variables on the highly entangled effect through the analysis of four molecular structures, aiming to design zwitterionic hydrogels with mechanical properties tailored to meet practical application requirements.

關鍵字(中)

★ 雙離子材料
★ 水凝膠
★ 高度纏結
★ 網絡均勻度
★ 表面吸附能
★ 非特異性吸附

關鍵字(英)

★ zwitterionic materials
★ hydrogels
★ high entanglement
★ network homogeneity
★ surface adsorption energy
★ anit-nonspecific adsorption

論文目次

目錄
中文摘要 I
Abstract III
致謝 V
目錄 VI
圖目錄 IX
表目錄 X
化學品名詞代稱 XI
產物名詞代稱 XII
一、文獻回顧 1
1-1 水凝膠之概述 1
1-2 防汙材料之發展 2
1-3 雙離子材料 4
1-3-1 雙離子材料之應用 5
1-3-2 雙離子水凝膠之缺陷 6
1-4 改善水凝膠機械性質之研究發展 6
1-4-1 互穿聚合物網絡(IPNs) 7
1-4-2 雙層網絡水凝膠(DN) 7
1-4-2 奈米複合水凝膠 9
1-4-3 奈米複合水凝膠 10
1-5 水凝膠之主要交聯方式 11
1-5-1 疏水相互作用之物理交聯 12
1-5-2 結晶之物理交聯 13
1-5-3 氫鍵之物理交聯 13
1-5-4 光聚合之化學交聯 14
1-5 高度纏結水凝膠之研究 15
二、研究目的 17
三、實驗藥品與實驗方法 18
3-1 實驗藥品 18
3-2 實驗設備 19
3-3 材料製備 20
3-3-1 Sulfobetaine methacrylate ,(SBMA)單體合成 20
3-3-2 Sulfobetaine acrylate ,(SBA)單體合成 20
3-3-3 Sulfobetaine acrylamide ,(SBAA)單體合成 21
3-3-4 Sulfobetaine methacrylamide ,(SBMAA)單體合成 21
3-3-4 水凝膠 / 聚合物製備 22
3-3-5 水凝膠對玻璃表面修飾樣品製備 23
3-4 實驗方法 24
3-4-1 液態核磁共振光譜儀鑑定(1H NMR) 24
3-4-2 準一級聚合反應測試(Pseudo-first-order polymerization kinetics) 24
3-4-3 機械性質-拉伸測試 25
3-4-4 遲滯現象測試-拉伸測試 25
3-4-5 流變儀(Rheometer) 25
3-4-6 衰減全反射式傅立葉轉換紅外線光譜儀分析(ATR-FTIR) 26
3-4-7膨潤度以及韌性增加率關係測試 26
3-4-8交聯密度測試-壓縮測試 27
3-4-9壓縮測試-貼附能測試 27
3-4-10動態光散射儀(DLS) 28
3-4-11表面吸附能測試-原子力顯微鏡(AFM) 29
3-4-12水下摩擦力測試-拉伸測試 30
3-4-13蛋白質貼附測試(Protein Adsorption Test) 31
3-4-14細菌貼附測試(Bacterial Adsorption Test) 32
3-4-15統計分析 32
四、結果與討論 33
4-1 單體結構與高度纏結雙離子水凝膠比例之鑑定 33
4-1-1 Sulfobetaine acrylate (SBA)1H NMR光譜鑑定 33
4-1-2 Sulfobetaine methacrylate (SBMA) 1H NMR光譜鑑定 35
4-1-3 Sulfobetaine acrylamide (SBAA)單體1H NMR光譜鑑定 37
4-1-4 Sulfobetaine methacrylamide (SBMAA)單體1H NMR光譜鑑定 39
4-2 雙離子水凝膠機械性質分析 41
4-2-1 高度纏結雙離子水凝膠比例鑑定 41
4-2-2 雙離子水凝膠機械性質之比較 43
4-3 氫鍵作用力與水合能力測試 46
4-3-1 雙離子水凝膠之FTIR圖譜分析 46
4-3-2 膨潤度與機械性質分析 48
4-4 水凝膠網絡均勻度分析 49
4-5 表面性質分析 57
4-5-1 水下潤滑度分析 57
4-5-2 表面吸附能分析 59
4-5-3 表面貼附應力測試 60
4-6-1 水凝膠貼附測試 61
五、結論 64
六、未來展望 66
七、參考文獻 67

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指導教授

黃俊仁(Chun-Jen Huang)

審核日期

2024-7-18

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