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標題: | 添加石墨烯之羥丙基甲基纖維素/幾丁聚醣/聚氧化乙烯電紡複合纖維膜製備及其特性探討 Fabrication and Characterization of Hydroxypropyl methylcellulose/Chitosan/Polyethylene oxide Electrospun Nanofiber Membranes Embedded with Graphene |
作者: | Li-Chang Cheng 鄭立昌 |
指導教授: | 謝學真(Hsyue-Jen Hsieh) |
關鍵字: | 靜電紡絲法,羥丙基甲基纖維素,幾丁聚醣,石墨烯,聚氧化乙烯,緻密膜,抗細胞貼附,膨潤度,藥物釋放,細菌貼附,水氣透過率, electrospinning,hydroxypropyl methylcellulose,chitosan,graphene,polyethylene oxide,anti-cell adhesion,,swelling ratio,antibacterial,water vapor transmission rate, |
出版年 : | 2018 |
學位: | 碩士 |
摘要: | 奈米纖維膜具有高比表面積、高質傳速率、孔洞小等特性,應用於傷口敷料上能快速止血、有效吸收滲液、維持良好水氣通透度與阻擋細菌侵入。本研究以靜電紡絲法(簡稱電紡)製備奈米纖維膜,材料選用羥丙基甲基纖維素(H)、幾丁聚醣(C)、石墨烯(G)和聚氧化乙烯(P),其中前兩者為天然材料,用以提高膜材親水性、膨潤性、抗菌性和生物相容性,而石墨烯作為抗菌奈米材料,聚氧化乙烯則為幫助電紡的超高分子量材料。本研究先探討最佳電紡參數,並分析纖維結構與孔洞大小、機械性質、水相環境穩定度、親水性、膨潤性與透水氣性等,再進行應用測定包括抗細胞貼附性、細胞毒性與抗菌性等,以期了解此電紡纖維膜是否具備成為抗菌生醫敷料的潛力。
本研究配製了不同成分比例的羥丙基甲基纖維素/幾丁聚醣/聚氧化乙烯(HCP)電紡溶液,以不同溶液流量、電壓電紡成為HCP纖維膜,並利用溶液性質分析與SEM圖觀察纖維型態。研究結果發現,當HCP三種材料總濃度為9.75 wt% (H:4.5 wt%, C:4.5 wt%, P:0.75 wt%),溶劑中醋酸濃度為25 wt%,能製備出型態良好的HCP纖維膜,再添加石墨烯成為HCPG纖維膜並大量製備,做後續性質和應用測試。 為提高纖維膜穩定性,將HCPG纖維膜以戊二醛(GA)進行不同時間下的蒸氣交聯,並進行機械性質與崩解性測定,由機械性質測定結果可知,HCPG纖維膜最佳交聯時間為2小時,其抗拉強度為1.38 ± 0.06 MPa。崩解性測定結果可知,以戊二醛交聯2小時的HCPG纖維膜,浸泡於磷酸緩衝溶液14天後能維持良好纖維型態。氣泡接觸角法測定膜材親水性,因為羥丙基甲基纖維素具有高親水性,使HCPG纖維膜親水性優於市售傷口敷料。 纖維膜應用方面,由纖維直徑與孔洞大小分析可知,HCPG纖維膜的纖維直徑為293 ± 235 nm,孔洞大小為1.16 ± 1.45 μm,較大部分細菌為小,不利於細菌貼附與穿透。由膜材膨潤度結果可知,添加羥丙基甲基纖維素的膜材吸水能力提升,使戊二醛交聯後的HCPG纖維膜膨潤度穩定值為1329.1 ± 43.2 %。透水氣測定結果可知,HCPG纖維膜於濕潤狀態下的水氣透過率(WVTR)為3129 g/m2 - day,接近燒燙傷敷料的建議水氣透過率,未來還可透過與不同膜材結合的方式來調整水氣透過率,以符合各種應用需求。再以纖維母細胞進行纖維膜的抗細胞貼附性測定與細胞毒性測定,實驗顯示細胞不易貼附於膜材上,且浸泡過纖維膜的培養液並無細胞毒性。再以大腸桿菌(E. coli)進行膜材抗菌性測試,由細菌貼附測定結果可知,短時間高濃度菌液培養下,HCP纖維膜抗菌效果優於3M人工皮與幾丁聚醣緻密膜,添加石墨烯後成為HCPG纖維膜,則其抗菌效果更明顯提升,且纖維膜孔洞小的特性也能阻擋細菌侵入,透過定時更換敷料能將細菌移除。 本研究製備的電紡纖維膜具良好機械強度,其親水性優於市售敷料與純幾丁聚醣纖維膜,並具有高吸水能力,有助於吸收組織滲液,透水氣速率也接近燒燙傷建議值,未來還可透過與不同膜材結合的方式,來調整透水氣速率,以符合各種應用需求。此外,纖維膜具有抗細胞貼附性與無細胞毒性,添加石墨烯後更提升抗菌效果,由此可知,本研究製備出的HCP及HCPG電紡複合纖維膜具有發展為抗菌生醫敷料的潛力。 Nanofiber membranes have favorable characteristics such as high specific surface area, high mass transfer rate and small pore size. They can be used as wound dressings for rapid hemostasis, absorbing wound exudate, suitable water vapor transmission and blocking invasion of bacteria. In this research, nanofiber membranes were fabricated by electrospinning. Hydroxypropyl methylcellulose (HPMC, H), chitosan (C) and graphene (G) were chosen as membrane materials to increase the hydrophilicity, swelling ratio and antibacterial property of the membrane. In addition, polyethylene oxide (PEO, P) was added to improve the yield of nanofibers. The optimal parameters for electrospinning, microsturcture, mechanical properties, stability, hydrophilicity, swelling ratio, water vapor transmission rate of the membranes were investigated. Moreover, anti-cell adhesion properties, cytotoxicity and antibacterial properties of the membranes were analyzed to evaluate their potential as antibacterial wound dressings. Various HCP solutions were prepared and electrospun into nanofibers under different electrospinning conditions. As indicated by SEM, the HCP solution with total material concentration of 9.75 wt% (H : 4.5 wt%, C : 4.5 wt%, P : 0.75 wt%) prepared in a 25 wt% acetic acid solution as the solvent could be electrospun into HCP nanofiber membrane with good fiber structure. In some experiments, graphene was added to fabricate HCPG nanofiber membrane. To improve the stability of nanofiber membranes, the membranes were crosslinked by glutaraldehyde (GA) vapor. The optimal GA crosslinking time of HCPG membrane was 2 hours and the tensile strength of the membrane was 1.38 ± 0.06 MPa. The membrane stability test showed that the morphology and weight of the membranes could be maintained after immersion in PBS for 14 days. The hydrophilicity test showed that HCPG membrane was more hydrophilic than several commercial wound dressings. The fiber diameter of HCPG membrane was 293 ± 235 nm and the pore size was 1.16 ± 1.45 μm, both values smaller than the sizes of most bacteria. Hence, the microstructure of membrane could keep bacteria from adhesion and penetration. The swelling ratio of crosslinked HCPG membrane was 1329.1 ± 43.2 %. The water vapor transmission rate (WVTR) of wet HCPG membrane was 3129 g/m2 - day, close to the recommended WVTR of wound dressings. The anti-cell adhesion property and cytotoxicity tests showed that it was difficult for fibroblasts to attach to the membrane which had no cytotoxicity. The assay of bacterial adhension showed the antibacterial effect of HCP membrane was better than 3M Tegaderm artificial skin and chitosan dense film. As compared with HCP membrane, the antibacterial effect of HCPG membrane was even better. Besides, the small pore sizes of nanofiber membrane could keep bacteria from penetration into the membrane. The HCPG nanofiber membrane had good mechanical properties and hydrophilicity. The high water uptake capability of HCPG membrane could be used to absorb wound exudate. The WVTR of the membrane was approximately in the WVTR range of commercial wound dressings. Besides, HCPG membrane exhibited anti-cell adhesion, nontoxic, and antibacterial properties. Therefore, HCP and HCPG nanofiber membranes have the potential to become antibacterial wound dressings. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/77778 |
DOI: | 10.6342/NTU201801759 |
全文授權: | 有償授權 |
電子全文公開日期: | 2023-07-25 |
顯示於系所單位: | 化學工程學系 |
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