| 研究生: |
游智戎 You, Zhi-Rong |
|---|---|
| 論文名稱: |
以同軸電紡製備聚癸二酸丙三醇酯纖維薄膜與其機械特性之探討 Fabrication of poly(glycerol sebacate) fibrous membranes by coaxial electrospinning and characterization of their mechanical properties |
| 指導教授: |
胡晉嘉
Hu, Jin-Jia |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 生物醫學工程學系 Department of BioMedical Engineering |
| 論文出版年: | 2015 |
| 畢業學年度: | 103 |
| 語文別: | 中文 |
| 論文頁數: | 80 |
| 中文關鍵詞: | 同軸靜電紡絲 、PGS纖維薄膜 、機械性質 |
| 外文關鍵詞: | Coaxial electrospinning, PGS fibrous membrane, mechanical properties |
| 相關次數: | 點閱:115 下載:0 |
| 分享至: |
| 查詢本校圖書館目錄 查詢臺灣博碩士論文知識加值系統 勘誤回報 |
本研究使用兩種天然單體所合成出來的聚癸二酸丙三醇酯(poly(glycerol sebacate),PGS)彈性體,其生物可降解性且富有良好的彈性,然而,對於製備出PGS奈米纖維有著一大挑戰,無論是PGS prepolymer,由於其分子量低,分子間的交纏程度不夠,或是交聯後的PGS彈性體,無法有合適的溶劑配製成電紡溶液,皆有著單獨電紡出PGS纖維之困難性。在本研究中使用客製化的同軸電紡裝置,透過已知可電紡之高分子材料做為外管帶出內管不可紡之高分子材料(PGS prepolymer),製備出具芯/殼結構之電紡纖維薄膜,使用PLA做為外管材料因為其熔點能夠承受內管PGS交聯溫度,特別的是探討在外管溶液中添加PEO,在交聯之前將PEO移除,對於薄膜之影響。使用穿透式顯微鏡確認同軸纖維之芯-殼結構;掃描式顯微鏡觀察電紡薄膜的表面形態,添加PEO纖維直徑是減小的;移除外管材料的過程可以透過傅立葉轉換紅外線光譜來確認纖維薄膜的官能基,將纖維薄膜放入真空烘箱在不同的交聯溫度與時間進行交聯反應,使用單軸拉伸測試得知纖維薄膜的機械性質,與先前研究相同的是,隨著交聯溫度的提高與時間的增加,薄膜的楊氏模數與拉伸強度隨之上升,剛性(stiffness)增加;有趣的是,外管的PLA材料對於具PGS/PLA芯/殼結構之電紡纖維薄膜的機械性質來說扮演重要的角色,外管溶液為PEO/PLA混合溶液相較於純PLA是更有柔順性;提高內管溶液的PGS濃度,纖維薄膜的剛性增強,讓內管PGS有主導纖維薄膜機械性質之能力;最後以70% PGS為內管溶液,PEO/PLA混合溶液為外管溶液所製備具PGS/PLA芯/殼結構之電紡纖維薄膜移除外管PLA材料後,得到PGS電紡纖維薄膜,根據交聯的條件楊氏模數範圍約為0.47~1.03MPa,其機械性質有較佳的柔順性與彈性,能夠運於軟組織範圍中,並且證實以高度順向性的PGS纖維對平滑肌細胞有產生接觸引導(contact guidance)的能力,以此PGS纖維製作的組織工程支架,有著類似於細胞外基質的結構,有潛力可成為軟組織工程支架。
It is challenging to fabricate electrospun PGS nanofibers because of the poor electrospinnability of its prepolymer and fully crosslinked polymer the low molecular weight. In this study, coaxial electrospinning, which allows a non-electrospinnable polymer to be drawn by a electrospinnable polymer was used aiming at fabricate PGS nanofibers. PLA was used as shell material because it does not melt at PGS curing temperature confining PGS prepolymer in the core. Specifically, the effects of adding PEO in the shell solution were investigated; PEO was removed prior to curing. The fibrous membranes were cured in a vacuum oven at varying temperatures for different reaction time. Transmission electron microscopy was used to illustrate core-shell structure of the fibers. Scanning electron microscopy was used to examine the morphology of membranes. Fourier transform infrared spectroscopy was used to confirm functional group of the membrane after removing PEO and PLA shell. Mechanical properties of the membrane were examined by uniaxial tensile testing. The addition of PEO decreased the fiber diameter. Consistent with previous studies, we found that both the higher curing temperature and the longer duration of curing increased the stiffness of the membrane. We found that PLA appeared to play a role in the mechanical properties of electrospun PGS membrane. The electrospun core/shell PGS/PLA membranes fabricated with PEO/PLA mixture as shell material are more compliant. Moreover, increasing the PGS concentration in the core, the electrospun membrane became stiffer. The core seemed to dominate the mechanical properties of the membrane when 70% PGS was used as the core solution. Finally, electrospun PGS membrane with no PLA in the shell were achieved from the fibers fabricated with 70% PGS as the core solution and PEO/PLA mixture as the shell material. After the removal of PLA shell, PGS fibrous membrane was more compliant and had better flexibility. The Young’s modulus of electrospun PGS membrane was in the range of 0.47~1.03MPa, depending on curing conditions, which is similar to that of soft tissues. We also demonstrated by seeding smooth muscle cells on the membranes containing aligned fibers and found that they have potential of guiding cells alignment.
[1] R. Murugan and S. Ramakrishna, "Design strategies of tissue engineering scaffolds with controlled fiber orientation," Tissue Engineering, vol. 13, pp. 1845-1866, Aug 2007.
[2] Q. Chen, S. Liang, and G. A. Thouas, "Elastomeric biomaterials for tissue engineering," Progress in polymer science, vol. 38, pp. 584-671, 2013.
[3] Q. P. Pham, U. Sharma, and A. G. Mikos, "Electrospinning of polymeric nanofibers for tissue engineering applications: a review," Tissue engineering, vol. 12, pp. 1197-1211, 2006.
[4] S. Sell, C. Barnes, M. Smith, M. McClure, P. Madurantakam, J. Grant, et al., "Extracellular matrix regenerated: tissue engineering via electrospun biomimetic nanofibers," Polymer International, vol. 56, pp. 1349-1360, 2007.
[5] R. Lanza, R. Langer, and J. P. Vacanti, Principles of tissue engineering: Academic press, 2011.
[6] S. Chung and M. W. King, "Design concepts and strategies for tissue engineering scaffolds," Biotechnology and applied biochemistry, vol. 58, pp. 423-438, 2011.
[7] C. Vaz, S. Van Tuijl, C. Bouten, and F. Baaijens, "Design of scaffolds for blood vessel tissue engineering using a multi-layering electrospinning technique," Acta biomaterialia, vol. 1, pp. 575-582, 2005.
[8] W. He, T. Yong, W. E. Teo, Z. Ma, and S. Ramakrishna, "Fabrication and endothelialization of collagen-blended biodegradable polymer nanofibers: potential vascular graft for blood vessel tissue engineering," Tissue engineering, vol. 11, pp. 1574-1588, 2005.
[9] J.-J. Hu, W.-C. Chao, P.-Y. Lee, and C.-H. Huang, "Construction and characterization of an electrospun tubular scaffold for small-diameter tissue-engineered vascular grafts: a scaffold membrane approach," Journal of the mechanical behavior of biomedical materials, vol. 13, pp. 140-155, 2012.
[10] Z.-M. Huang, Y.-Z. Zhang, M. Kotaki, and S. Ramakrishna, "A review on polymer nanofibers by electrospinning and their applications in nanocomposites," Composites science and technology, vol. 63, pp. 2223-2253, 2003.
[11] E. C. Novosel, C. Kleinhans, and P. J. Kluger, "Vascularization is the key challenge in tissue engineering," Advanced drug delivery reviews, vol. 63, pp. 300-311, 2011.
[12] Y. Wang, G. A. Ameer, B. J. Sheppard, and R. Langer, "A tough biodegradable elastomer," Nature biotechnology, vol. 20, pp. 602-606, 2002.
[13] H. Inoguchi, I. K. Kwon, E. Inoue, K. Takamizawa, Y. Maehara, and T. Matsuda, "Mechanical responses of a compliant electrospun poly(L-lactide-co-epsilon-caprolactone) small-diameter vascular graft," Biomaterials, vol. 27, pp. 1470-1478, Mar 2006.
[14] C. M. Chan, T. M. Ko, and H. Hiraoka, "Polymer surface modification by plasmas and photons," Surface Science Reports, vol. 24, pp. 3-54, 1996.
[15] P. K. Chu, J. Y. Chen, L. P. Wang, and N. Huang, "Plasma-surface modification of biomaterials," Materials Science & Engineering R-Reports, vol. 36, pp. 143-206, Mar 29 2002.
[16] Q.-Z. Chen, A. Bismarck, U. Hansen, S. Junaid, M. Q. Tran, S. E. Harding, et al., "Characterisation of a soft elastomer poly (glycerol sebacate) designed to match the mechanical properties of myocardial tissue," Biomaterials, vol. 29, pp. 47-57, 2008.
[17] C. A. Sundback, J. Y. Shyu, Y. Wang, W. C. Faquin, R. S. Langer, J. P. Vacanti, et al., "Biocompatibility analysis of poly (glycerol sebacate) as a nerve guide material," Biomaterials, vol. 26, pp. 5454-5464, 2005.
[18] Y. Kang, J. Yang, S. Khan, L. Anissian, and G. A. Ameer, "A new biodegradable polyester elastomer for cartilage tissue engineering," Journal of Biomedical Materials Research Part A, vol. 77, pp. 331-339, 2006.
[19] C. J. Bettinger, B. Orrick, A. Misra, R. Langer, and J. T. Borenstein, "Microfabrication of poly (glycerol–sebacate) for contact guidance applications," Biomaterials, vol. 27, pp. 2558-2565, 2006.
[20] F. Yi and D. A. LaVan, "Poly (glycerol sebacate) nanofiber scaffolds by core/shell electrospinning," Macromolecular bioscience, vol. 8, pp. 803-806, 2008.
[21] Huang and Z., "A review on polymer nanofibers by electrospinning and their applications in nanocomposites," Composites Science and Technology, vol. 63, pp. 2223-2253, 2003.
[22] W. E. Teo and S. Ramakrishna, "A review on electrospinning design and nanofibre assemblies," Nanotechnology, vol. 17, pp. R89-R106, Jul 28 2006.
[23] S. P. Zhong, W. E. Teo, X. Zhu, R. W. Beuerman, S. Ramakrishna, and L. Y. L. Yung, "An aligned nanofibrous collagen scaffold by electrospinning and its effects on in vitro fibroblast culture," Journal of Biomedical Materials Research Part A, vol. 79A, pp. 456-463, Dec 1 2006.
[24] A. Formhals, vol. US patent 1-975-504,1934.
[25] D. H. Reneker and I. Chun, "Nanometre diameter fibres of polymer, produced by electrospinning," Nanotechnology, vol. 7, pp. 216-223, Sep 1996.
[26] S. R. Bhattarai, N. Bhattarai, H. K. Yi, P. H. Hwang, D. I. Cha, and H. Y. Kim, "Novel biodegradable electrospun membrane: scaffold for tissue engineering," Biomaterials, vol. 25, pp. 2595-2602, 2004.
[27] A. Saraf, G. Lozier, A. Haesslein, F. K. Kasper, R. M. Raphael, L. S. Baggett, et al., "Fabrication of Nonwoven Coaxial Fiber Meshes by Electrospinning," Tissue Engineering Part C-Methods, vol. 15, pp. 333-344, Sep 2009.
[28] A. K. Moghe and B. S. Gupta, "Co-axial electrospinning for nanofiber structures: Preparation and applications," Polymer Reviews, vol. 48, pp. 353-377, 2008.
[29] Y. Su, X. Q. Li, H. S. Wang, C. L. He, and X. M. Mo, "Fabrication and characterization of biodegradable nanofibrous mats by mix and coaxial electrospinning," Journal of Materials Science-Materials in Medicine, vol. 20, pp. 2285-2294, Nov 2009.
[30] Y. Su, X. Li, H. Wang, C. He, and X. Mo, "Fabrication and characterization of biodegradable nanofibrous mats by mix and coaxial electrospinning," Journal of Materials Science: Materials in Medicine, vol. 20, pp. 2285-2294, 2009.
[31] C. Wang, K.-W. Yan, Y.-D. Lin, and P. C. Hsieh, "Biodegradable core/shell fibers by coaxial electrospinning: processing, fiber characterization, and its application in sustained drug release," Macromolecules, vol. 43, pp. 6389-6397, 2010.
[32] M. G. McKee, G. L. Wilkes, R. H. Colby, and T. E. Long, "Correlations of solution rheology with electrospun fiber formation of linear and branched polyesters," Macromolecules, vol. 37, pp. 1760-1767, Mar 9 2004.
[33] H. Fong, I. Chun, and D. H. Reneker, "Beaded nanofibers formed during electrospinning," Polymer, vol. 40, pp. 4585-4592, Jul 1999.
[34] L. Huang, Nagapudi, Karthik, P.Apkarian, Robert, Chaikof, et al., "Engineered collagen-PEO nanofibers and fabrics," Journal of Biomaterials Science, Polymer Edition, vol. 12, pp. 979-993, 2001.
[35] H. Jiang, D. Fang, B. S. Hsiao, B. Chu, and W. Chen, "Optimization and Characterization of Dextran Membranes Prepared by Electrospinning," Biomacromolecules, vol. 5, pp. 326-333, 2004.
[36] C. Ki, D. Baek, K. Gang, K. Lee, I. Um, and Y. Park, "Characterization of gelatin nanofiber prepared from gelatin–formic acid solution," Polymer, vol. 46, pp. 5094-5102, 2005.
[37] X. Zong, K. Kim, D. Fang, S. Ran, B. S. Hsiao, and B. Chu, "Structure and process relationship of electrospun bioabsorbable nanofiber membranes," Polymer, vol. 43, pp. 4403-4412, 2002.
[38] W. Zuo, M. Zhu, W. Yang, H. Yu, Y. Chen, and Y. Zhang, "Experimental study on relationship between jet instability and formation of beaded fibers during electrospinning," Polymer Engineering & Science, vol. 45, pp. 704-709, 2005.
[39] Z. Huang, "A review on polymer nanofibers by electrospinning and their applications in nanocomposites," Composites Science and Technology, vol. 63, pp. 2223-2253, 2003.
[40] C. J. Buchko, L. C. Chen, Y. Shen, and D. C. Martin, "Processing and microstructural characterization of porous biocompatible protein polymer thin films," Polymer, vol. 40, pp. 7397-7407, 1999.
[41] Z. Jun, H. Q. Hou, A. Schaper, J. H. Wendorff, and A. Greiner, "Poly-L-lactide nanofibers by electrospinning - Influence of solution viscosity and electrical conductivity on fiber diameter and fiber morphology," E-Polymers, 2003.
[42] Y. J. Ryu, H. Y. Kim, K. H. Lee, H. C. Park, and D. R. Lee, "Transport properties of electrospun nylon 6 nonwoven mats," European Polymer Journal, vol. 39, pp. 1883-1889, 2003.
[43] H. Chen and Y. L. Hsieh, "Ultrafine hydrogel fibers with dual temperature- and pH-responsive swelling behaviors," Journal of Polymer Science Part a-Polymer Chemistry, vol. 42, pp. 6331-6339, Dec 15 2004.
[44] Koski and A., "Effect of molecular weight on fibrous PVA produced by electrospinning," Materials Letters, vol. 58, pp. 493-497, 2004.
[45] B. Kim, H. Park, S. H. Lee, and W. M. Sigmund, "Poly(acrylic acid) nanofibers by electrospinning," Materials Letters, vol. 59, pp. 829-832, Mar 2005.
[46] M. M. Demir, I. Yilgor, E. Yilgor, and B. Erman, "Electrospinning of polyurethane fibers," Polymer, vol. 43, pp. 3303-3309, May 2002.
[47] T. Jarusuwannapoom, W. Hongrojjanawiwat, S. Jitjaicham, L. Wannatong, M. Nithitanakul, C. Pattamaprom, et al., "Effect of solvents on electro-spinnability of polystyrene solutions and morphological appearance of resulting electrospun polystyrene fibers," European Polymer Journal, vol. 41, pp. 409-421, 2005.
[48] H. S. Kim, K. Kim, H. J. Jin, and I.-J. Chin, "Morphological Characterization of Electrospun Nano-Fibrous Membranes of Biodegradable Poly(L-lactide) and Poly(lactide-co-glycolide)," Macromolecular Symposia, vol. 224, pp. 145-154, 2005.
[49] J. S. Lee, K. H. Choi, H. Do Ghim, S. S. Kim, D. H. Chun, H. Y. Kim, et al., "Role of molecular weight of atactic poly(vinyl alcohol) (PVA) in the structure and properties of PVA nanofabric prepared by electrospinning," Journal of Applied Polymer Science, vol. 93, pp. 1638-1646, 2004.
[50] L. Wannatong, A. Sirivat, and P. Supaphol, "Effects of solvents on electrospun polymeric fibers: preliminary study on polystyrene," Polymer International, vol. 53, pp. 1851-1859, 2004.
[51] X. Yuan, Y. Zhang, C. Dong, and J. Sheng, "Morphology of ultrafine polysulfone fibers prepared by electrospinning," Polymer International, vol. 53, pp. 1704-1710, 2004.
[52] X. Geng, O. Kwon, and J. Jang, "Electrospinning of chitosan dissolved in concentrated acetic acid solution," Biomaterials, vol. 26, pp. 5427-5432, 2005.
[53] Z. Zhao, J. Li, X. Yuan, X. Li, Y. Zhang, and J. Sheng, "Preparation and properties of electrospun poly(vinylidene fluoride) membranes," Journal of Applied Polymer Science, vol. 97, pp. 466-474, 2005.
[54] N. L'Heureux, S. Paquet, R. Labbe, L. Germain, and F. A. Auger, "A completely biological tissue-engineered human blood vessel," Faseb Journal, vol. 12, pp. 47-56, Jan 1998.
[55] K. H. Lee, H. Y. Kim, H. J. Bang, Y. H. Jung, and S. G. Lee, "The change of bead morphology formed on electrospun polystyrene fibers," Polymer, vol. 44, pp. 4029-4034, Jun 2003.
[56] 王盈淇, "溫度效應對電紡絲製備高分子纖維之影響," 碩士, 化學工程學系, 國立成功大學, 2004.
[57] K. M. Nampoothiri, N. R. Nair, and R. P. John, "An overview of the recent developments in polylactide (PLA) research," Bioresource technology, vol. 101, pp. 8493-8501, 2010.
[58] Y. Li and H. Shimizu, "Toughening of polylactide by melt blending with a biodegradable poly (ether) urethane elastomer," Macromolecular bioscience, vol. 7, pp. 921-928, 2007.
[59] C.-C. Chen, J.-Y. Chueh, H. Tseng, H.-M. Huang, and S.-Y. Lee, "Preparation and characterization of biodegradable PLA polymeric blends," Biomaterials, vol. 24, pp. 1167-1173, 2003.
[60] N. P. Desai and J. A. Hubbell, "Solution technique to incorporate polyethylene oxide and other water-soluble polymers into surfaces of polymeric biomaterials," Biomaterials, vol. 12, pp. 144-153, 1991.
[61] H. Tadokoro, Y. Chatani, T. Yoshihara, S. Tahara, and S. Murahashi, "Structural studies on polyethers,[‐(CH2) m‐O‐] n. II. Molecular structure of polyethylene oxide," Die Makromolekulare Chemie, vol. 73, pp. 109-127, 1964.
[62] E. Martuscelli, Polymer Blends: Processing, Morphology, and Properties: Springer Science & Business Media, 2012.
[63] B. Xu, B. Rollo, L. A. Stamp, D. Zhang, X. Fang, D. F. Newgreen, et al., "Non-linear elasticity of core/shell spun PGS/PLLA fibres and their effect on cell proliferation," Biomaterials, vol. 34, pp. 6306-6317, 2013.
[64] M. C. Wake, P. K. Gupta, and A. G. Mikos, "Fabrication of pliable biodegradable polymer foams to engineer soft tissues," Cell transplantation, vol. 5, pp. 465-473, 1996.
[65] J. J. Hu, W. C. Chao, P. Y. Lee, and C. H. Huang, "Construction and characterization of an electrospun tubular scaffold for small-diameter tissue-engineered vascular grafts: a scaffold membrane approach," J Mech Behav Biomed Mater, vol. 13, pp. 140-55, Sep 2012.
[66] A. Koski, K. Yim, and S. Shivkumar, "Effect of molecular weight on fibrous PVA produced by electrospinning," Materials Letters, vol. 58, pp. 493-497, Jan 2004.
[67] C. Ribeiro, V. Sencadas, C. Caparrós, J. Ribelles, and S. Lanceros-Méndez, "Fabrication of Poly (lactic acid)-Poly (ethylene oxide) Electrospun Membranes with Controlled Micro to Nanofiber Sizes," Journal of nanoscience and nanotechnology, vol. 12, pp. 6746-6753, 2012.
[68] H. Zhou, "Electrospun fibers from both solution and melt: Processing, structure and property," Cornell University, 2007.
[69] B. Xu, Y. Li, X. Fang, G. A. Thouas, W. D. Cook, D. F. Newgreen, et al., "Mechanically tissue-like elastomeric polymers and their potential as a vehicle to deliver functional cardiomyocytes," Journal of the mechanical behavior of biomedical materials, vol. 28, pp. 354-365, 2013.
[70] E. D. Boland, G. E. Wnek, D. G. Simpson, K. J. Pawlowski, and G. L. Bowlin, "Tailoring tissue engineering scaffolds using electrostatic processing techniques: a study of poly (glycolic acid) electrospinning," Journal of Macromolecular Science, Part A, vol. 38, pp. 1231-1243, 2001.
[71] S. Elsevier, "Journal of the Mechanical Behavior of Biomedical Materials," 收錄起迄年: 2007-Present, 2009.
[72] Y. Li, G. A. Thouas, and Q. Chen, "Novel elastomeric fibrous networks produced from poly (xylitol sebacate) 2: 5 by core/shell electrospinning: Fabrication and mechanical properties," Journal of the mechanical behavior of biomedical materials, vol. 40, pp. 210-221, 2014.
[73] J. Gao, P. M. Crapo, and Y. Wang, "Macroporous elastomeric scaffolds with extensive micropores for soft tissue engineering," Tissue engineering, vol. 12, pp. 917-925, 2006.
[74] Y. Wang, "Biorubber/poly (glycerol sebacate)," Informa Healthcare, London, pp. 121-128, 2004.
[75] R. Rai, M. Tallawi, A. Grigore, and A. R. Boccaccini, "Synthesis, properties and biomedical applications of poly (glycerol sebacate)(PGS): a review," Progress in Polymer Science, vol. 37, pp. 1051-1078, 2012.
校內:2020-09-30公開