透過貽貝啟發快速沉積的複合材料與結合兩性離子修飾方式發展具有抗菌及抗汙功能之通用表面塗層研究

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姓名

范玉珍(Yu-Jhen Fan) 查詢紙本館藏

畢業系所

生物醫學工程研究所

論文名稱

透過貽貝啟發快速沉積的複合材料與結合兩性離子修飾方式發展具有抗菌及抗汙功能之通用表面塗層研究
(Development of antimicrobial and antifouling universal coating via rapid deposition of composite mussel-inspired film and post-conjugation of zwitterionic moiety)

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摘要(中)

生物汙染是蛋白質、細胞或細菌等非特異性吸附於表面上，進而而形成血栓和生物膜。本研究提出一種通用基材表面修飾方式，使表面同時具有抵抗非特異性吸附，及抗菌的功能。本研究利用CuSO4及H2O2加速多巴胺的聚合與沉積速率，使表面於短時間內形成聚多巴胺層，且可同時螯合溶液中的銅離子(Cu2+)於表面上，並藉由銅離子釋放達到殺菌效果。形成的pDA功能薄膜後，再藉由aza-Michael addition反應方式接枝雙離子材料丙烯醯胺磺基甜菜鹼 (sulfobetaine acrylamide，SBAA)，形成具有超親水之抗非特異性貼附之生物界面。利用接觸角測角儀 (contact angle) 進行表面鑑定，在接枝SBAA後的條件下，表面水接觸角約為5度，具有良好的親水性質。在X射線光電子能譜儀 (x-ray photoelectron spectroscopy)顯示，修飾後的表面上，具有銅離子及SBAA的元素組態。而於細菌貼附實驗測試，經SBAA修飾後，可抵抗約90%、95%的大腸桿菌(E-coli)及表皮葡萄球菌(S.epidermidis)之貼附，且其中80%為死菌。最後將材料修飾於尿導管表面上，並由此證明，藉由銅離子的釋放達到抗菌的效果，且修飾後的表面具有良好抗細菌貼附特性。本研究開發無表面選擇之生物啟發抗菌塗層，不但可抵抗細菌的非特異性貼附(antifouling)，更利用銅離子作為殺菌劑，成為雙重功能(antifouling與antimicrobial)之萬用生物界面塗層，期待開發多功能生物界面且應用於醫療器材表面塗層，以提升其生物相容性與使用安全性。

摘要(英)

The formation of bacterial biofilms on indwelling medical devices generally causes high risks for adverse complications such as catheter-associated urinary tract infections. In this study, we report a simple, rapid approach to imparting durable antibacterial properties to various surfaces. Initially, we use CuSO4/H2O2 to accelerate the polymerization of dopamine and the deposition rate of polydopamine. The pDA-assisted immobilization of copper ions enables the surfaces to incorporate antimicrobial agents for adsorbed and planktonic bacteria. Then, the fouling properties were achieved by grafting zwitterionic sulfobetaine acrylamide (SBAA) onto the pDA ﬁlms via the aza-Michael addition. The surface chemical compositions upon pDA modiﬁcation and subsequent conjugation were monitored with X-ray photoelectron spectroscopy (XPS) and water contact angle measurements. Antifouling properties of coatings were challenged by Escherichia coli and Staphylococcus epidermidis. The results show that pDA coatings grafted with SBAA exhibited superhydrophilicity and excellent fouling resistance. In addition, copper ions exhibit excellent antibacterial activity. The composite coatings allowed reduction of adsorption of Escherichia coli and S.epidermidis by 90% and 95%, respectively, while appearing up to 80% of dead bacteria upon the release of copper ions as measured by inductively coupled plasma mass spectrometry. Moreover, the composite coatings have been applied on the silicone-based urinary catheters to avoid the growth of bacteria and infection. Consequently, we have presented a facile and universal approach to modify surfaces and accordingly providing antibacterial properties. This strategy provides a useful route to mitigating the long-term biofouling of various surfaces.

關鍵字(中)

★ 兩性離子
★ 多巴胺
★ 金屬離子
★ 抗非特異性吸附
★ 抗菌

關鍵字(英)

★ zwitterionic material
★ dopamine
★ non-specific adsorption
★ antimicrobials

論文目次

摘要 V
ABSTRACT VI
謝誌 VII
目錄 VIII
圖目錄 XI
表目錄 XV
簡寫對照表 XVI
第一章文獻回顧 1
1-1生物汙染 1
1-2生物膜形成機制 2
1-3醫療器材之生物汙染 3
1-4 抗生物汙染之生物塗層 4
1-4-1聚乙二醇材料 4
1-4-2雙離子材料 5
1-4-2-1 Phosphatidylcholine (PC)類雙離子材料 6
1-4-2-2 Sulfobetaine(SB)類雙離子材料 8
1-4-2-3 Carboxybetaine(CB)類雙離子材料 9
1-5表面修飾技術 10
1-5-1 高分子刷 10
1-5-2 自組裝單層膜 12
1-6 生物啟發之仿生材料 16
1-6-1貽貝蛋白 16
1-6-2多巴胺分子 17
1-6-3多巴胺分子的結構特性 18
1-6-4聚多巴胺的製備及形成機制 18
1-6-5聚多巴胺的表面功能化接枝及應用 22
1-6-6表面接枝胺基、硫醇分子 22
1-6-7 聚多巴胺與金屬離子之螯合 24
1-7抗微生物表面塗層 25
第二章研究目的 26
第三章實驗藥品、設備及實驗方法 28
3-1實驗藥品 28
3-2實驗設備 29
3-3實驗方法 30
3-3-1實驗架構圖 30
3-3-2實驗流程圖 31
3-3-3利用CuSO4/H2O2 觸發聚多巴胺於表面之修飾 31
3-3-4丙烯醯胺磺基甜菜鹼(SBAA)接枝方法 31
3-3-5接觸角測量(Contact angle) 32
3-3-6橢圓偏光儀(Ellipsometry) 32
3-3-7紫外-可見分光光度計(UV-Vis) 32
3-3-8高解析電子能譜儀(XPS)分析 32
3-3-9原子力顯微镜(AFM)分析: 33
3-3-10感應偶和電漿質譜儀 (ICP-MS) 33
3-3-11細菌貼附測量 33
3-3-12尿導管之抗菌測試 34
第四章實驗結果與討論 35
4-1表面元素組態及物理性質鑑定 35
4-1-1薄膜水接觸角測試 35
4-1-2 薄膜厚度測試 36
4-1-3 薄膜可見光紫外光分光光譜儀測量 37
4-1-4 XPS元素組成與薄膜之化學狀態 38
4-1-5薄膜原子力顯微镜分析 44
4-2抗汙及抗菌特性之鑑定 45
4-2-1銅離子釋放測試 45
4-2-2 活菌與死菌於表面之測試 46
4-3醫療器材實施 49
4-3-1通用塗層水接觸角測試 49
4-3-2通用塗層抗沾黏測試 51
4-3-3尿導管表面塗層之修飾 55
結論與未來展望 57
參考文獻 58

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指導教授

黃俊仁(Chun-Jen Huang)

審核日期

2017-6-26

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