生物可分解性聚(左旋乳酸)氨基甲酸酯之合成及性質探討

本研究以二步法合成出H or L/聚(左旋乳酸)氨基甲酸酯共聚合體，聚左旋乳酸二醇(Mw=3000)為軟鏈節與六亞甲基二異氰酸酯(HDI)或L-賴氨酸乙酯二異氰酸酯(LDI)作為硬鏈節進行預聚合反應，及鏈延長劑1,4丁二醇(BDO)進行合成。研究結果顯示，GPC分析確定其共聚合體重量平均分子量(Mw)分佈範圍為2.53×104 - 4.17×104，PDI為1.56-2.24。則由FT-IR與1H NMR確定聚合體結構。TGA探討聚合體的熱穩定性與衰解活化能，硬鏈節含量增加會改善聚合體的熱穩定性。藉由Ozawa法計算結果顯示，在各衰解階段的活化能H/PLAUs聚合體高於L/PLAUs聚合體。此外，TGA與Ozawa動力學分析顯示聚合體至少有兩個階段的衰解步驟產生。DSC結果顯示，聚合體的玻璃轉為溫度隨著硬鏈節含量增加而往高溫移動。XRD結果顯示，聚合體結晶度的增加會隨著硬鏈節含量增加。體外降解結果顯示，在12週的體外降解率L/PLAUs聚合體高於H/PLAUs聚合體。掃描式電子顯微鏡(SEM)結果顯示，表面形貌平滑的薄膜經過水解降解轉變成裂縫與孔洞。MTT細胞毒性測試顯示，聚合物薄膜材料生物毒性低，且具有良好的生物相容性。未來可應用於可吸收縫線、組織工程及藥物輸送系統等各種用途。

關鍵字

生物可分解性；聚左旋乳酸二醇；熱降解；體外降解

並列摘要

Poly(L-lactic acid)urethane copolymers were synthesized by two-step process. Poly(L-lactic acid)urethane copolymers prepared from poly(L-lactic acid) diol (PLLA diol) with a molecular weight 3000 which was used as a soft segment, Hexamethylene diisocyanate(HDI) or L-lysine ethyl ester diisocyanate(LDI) which was used as a hard segment to proceed pre-polymerization reaction, as take 1,4-butanediol (BDO) which was used as a chain extender to proceed the synthesis. The study result showed that gel permeation chromatography analysis determined the weight average molecular weights (Mw) were found in the range of 2.53×104 - 4.17×104 gmol-1 with polydispersity indexes (PDI) between 1.56 and 2.24. The spectrums of infrared and 1H NMR analysis determined the structure. The thermogravimetric analysis(TGA) was discussed thermal stability and activation energy of polymers. When the hard segment content increasel, the thermal stability of polymers improved. The activation energies at various degradation stages for the H/PLAUs and L/PLAUs polymers were calculated by the Ozawa method. The result showed that activation energies at various degradation stages of the H/PLAUs polymers were higher than those of L/PLUAs polymers. In addition, thermogravimetric analysis and Ozawa kinetic analysis revealed that at least two stages of degradation arise at these polymers. The differential scanning calorimetry(DSC) analyzer showed that glass temperature(Tg) of polymers increase along with ratio of hard segment content increased. X-ray diffraction(XRD) analyzer showed that crystallinity of polymers increase along with ratio of hard segment content increased. In vitro degradation result showed that the in vitro degradation rates of the L/PLAUs polymers were higher than those of H/PLUAs polymers during 12 weeks. Scanning electron microscope (SEM) observation results showed that the surface topography of the film was smooth, and transformed into holes and cracks through hydrolytic degradation. Furthermore, MTT cytotoxicity test showed good biocompatibility of the polymer film materials. It can be widely used in resorbable sutures, issue engineering and drug delivery systems in the future.

並列關鍵字

Biodegradable ； Poly(L-lactic acid) diol ； Thermal degradation ； In vitro degradation

參考文獻

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生物可分解性聚(左旋乳酸)氨基甲酸酯之合成及性質探討

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