提升抗菌性之四級銨鹽化幾丁聚醣合成及幾丁聚醣複合電紡纖維膜之製備與特性探討

本研究使用去乙醯度為91.7%之幾丁聚醣與縮水甘油基三甲基氯化銨(glycidyltrimethylammonium chloride, GTMAC)在純水中進行開環反應製備含有四級銨鹽官能基之水溶性幾丁聚醣(N-[(2-hydroxyl)-propyl-3-trimethylammonium] chitosan chloride, 簡稱HTCC)，並探討幾丁聚醣與GTMAC在不同反應條件與純化過程下之產率差異，再進一步使用FT-IR、NMR鑑定HTCC之分子結構；以導電度滴定法測定HTCC之取代度。實驗顯示反應體積161.857 ml、反應溫度85℃、GTMAC當量數為4，以及反應時間為6小時及8小時之HTCC產物，簡稱HTCC-6與HTCC-8具有較佳之產率、純度及胺基取代度。隨後配製分別含有HTCC-6與HTCC-8之電紡溶液，測量溶液黏度等性質，再將電紡溶液在不同製程參數下製成電紡纖維，並以SEM觀察纖維型態，探討電紡參數與溶液性質對於纖維型態的影響，找出適合大量製備電紡纖維的操作條件，其中組成為C2.5H2.5G5P0.5AA20-6之電紡溶液在電壓25 kV、溶液流量0.05 ml/min之的電紡條件下之纖維型態最佳。為提高纖維膜的穩定性，針對C2.5H2.5G5P0.5AA20-6纖維膜進行戊二醛蒸氣交聯，經探討發現交聯時間為1.5小時的纖維膜具有較佳的機械性質以及在水相環境中的穩定性。最後將交聯後的纖維膜進行抗菌性測試，結果發現纖維膜能在與大腸桿菌(菌株BL21(DE3))接觸的20小時內將細菌數減至極少，具有良好抗菌能力。本研究成功合成水溶性幾丁聚醣衍生物HTCC，也成功製備了含有HTCC之複合電紡纖維膜，並且證實此纖維膜對於大腸桿菌具有良好的抗菌能力，未來可將此含有四級銨鹽化幾丁聚醣(HTCC)複合電紡纖維膜發展成為抗菌性生醫材料。

關鍵字

幾丁聚醣；四級銨鹽化幾丁聚醣；靜電紡絲；抗菌材料

並列摘要

In this study, chitosan (degree of deacetylation: 91.7%) was used to react with glycidyltrimethylammonium chloride (GTMAC) to synthesize water-soluble chitosan — (N-[(2-hydroxyl)-propyl-3-trimethylammonium] chitosan chloride (HTCC), with quaternary salt functional groups. In addition, how the reaction yield and degree of substitution varied with reaction time and other reaction parameters were also investigated. The characteristics of HTCC were further examined by NMR, FT-IR and conductometric titration analysis. Eventually, two products (HTCC-6 and HTCC-8) had relatively better yields, purities and proper degree of substitutions. In order to find proper electrospinning parameters, various composite solutions containing HTCC-6 or HTCC-8 were prepared and used for fabrication of fibers by electrospinning device under different process parameters, such as applied voltage and solution flow rate. Based on the SEM images of these fibers, a solution named C2.5H2.5G5P0.5AA20-6 could be electrospun into fibers with desired morphologies under the conditions of applied voltage 25 kV and flow rate 0.05 ml/min. To increase the stability of fibers, the above-mentioned C2.5H2.5G5P0.5AA20-6 fibrous membrane was crosslinked by glutaraldehyde vapor. It was found that crosslinking time of 1.5 hours could enhance the tensile strength and stability of the fibrous membranes. The crosslinked membrane was subjected to in vitro antibacterial test. C2.5H2.5G5P0.5AA20-6 fibrous membrane was incubated with E. coli (strain BL21 (DE3)) for 20 hours and only very few bacteria survived on the fibrous membrane, indicating that C2.5H2.5G5P0.5AA20-6 fibrous membrane possessed great antibacterial activity against E. coli. at physiological pH (pH 7). In conclusion, the water-soluble chitosan derivative HTCC was successfully synthesized and used for fabrication of HTCC-containing composite electrospun fibrous membrane (C2.5H2.5G5P0.5AA20-6 membrane) which exhibited good antibacterial ability against E. coli, thus being a promising antibacterial biomaterial.

並列關鍵字

chitosan ； quaternized chitosan ； electrospinning ； antibacterial material

參考文獻

[1] Huang ZM, Zhang YZ, Kotaki M and Ramakrishna S. A review on polymer nanofibers by electrospinning and their applications in nanocomposites. Composites Science and Technology, 2003, 63(15), 2223-2253.

Google Scholar

[2] Ray SS, Chen SS, Li CW, Nguyenac NC, Nguyenac HT. A comprehensive review: electrospinning technique for fabrication and surface modification of membranes for water treatment application. RSC Advances, 2016, 6(88), 85495-85514.

Google Scholar

[3] Xue J, Wu T, Dai Y, Xia Y. Electrospinning and Electrospun Nanofibers: Methods, Materials, and Applications. Chemical Review, 2019, 119(8), 5298-5415.

Google Scholar

[4] Fong H, Chun I, Reneker DH. Beaded nanofibers formed during electrospinning. Polymer, 1999, 40(16), 4585-4592.

Google Scholar

[5] Reneker DH., Yarin AL, Fong H, Koombhongse S. Bending instability of electrically charged liquid jets of polymer solutions in electrospinning. Journal of Applied Physics, 2000, 87(9), 4531-4547.

Google Scholar

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提升抗菌性之四級銨鹽化幾丁聚醣合成及幾丁聚醣複合電紡纖維膜之製備與特性探討

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