本論文主要是針對全降解型生物可分解之聚酯類的聚乳酸(Poly lactic acid, PLA)/聚乙烯醇 ((poly(vinyl alcohol), PVA)、聚乳酸(Poly lactic acid, PLA)/聚己內酯 ( poly(ε-caprolactone), PCL) 合膠及在聚己內酯內混摻多壁奈米碳管 (multi-walled carbon nanotubes, MWNTs)在不同混掺配方下所得之合膠的抗張、熱學、結晶、微細結構等性質的研究討論。
首先，將PLA和PVA依不同比例熔融混摻製備成 PLAxPVAy合膠樣品。經扭矩(torque) 分析發現，PLAxPVAy合膠樣品所對應”穩定扭矩”與”穩定時間”隨PLA含量增加而明顯降低。經傅立葉紅外光譜 (Fourier-transform Infrared Spectrum, FTIR)觀測發現 ，隨PVA含量增加PLAxPVAy合膠樣品之羰基和羥基之振動吸收峰峰值，明顯向低波數位移；上述結果顯示此兩官能基會相互作用，有利於PLA及PVA分子相容性提昇。 再由DSC曲線、廣角X-射線繞射和偏光顯微鏡分析顯示，PVA可以作為成核劑促進PLA結晶。其中偏光顯微鏡分析觀察發現，經添加20 wt% PVA的PLA80PVA20合膠樣品其PLA球晶成長速率(spherulite growth rate)最快。 PLAxPVAy合膠樣品熱重示差分析（TGA）結果發現PLA80 PVA20合膠樣品”第二熱降解步驟”消失。
第二部份是將PLA和PCL依不同比例熔融混摻製備成 PLAx PCLy合膠樣品，並研究其抗張、熱學、結晶微細結構及光學等性質。從DSC分析結果顯示，PLA及PCL熔融溫度(Tm)會隨PLAxPCLy合膠中的PCL含量增加而靠近；且當PLA含量達70wt%時, PLA70PCL30合膠樣品之PLA及PCL 之Tm值最為靠近。上述結果推論PLA70PCL30合膠樣品內PLA與PCL分子間存在最大之交互作用力。 另結合動態力學分析和電子顯微鏡表面型態觀察結果揭示，PLA和PCL分子間僅能形成部份相容現象，在其非晶區中僅少量的PCL溶入PLA富相(PLA-rich phase)中，導致PLA玻璃轉移溫度（Tg）降低。 由偏光顯微鏡分析結果發現，在PLAxPCLy合膠樣品冷卻結晶過程中，PCL可能扮演成促進PLA的結晶的角色。 其中經添加30 wt% PCL的PLA70PCL30合膠樣品其PLA 球晶成長速率最快，所形成的PLA 球晶可達最大。最後由PLAxPCLy合膠樣品的機械性質顯示，可藉添加適量PCL將PLA的機械性質由脆性轉為韌性。
第三部分研究是用熔融混摻的方法製備PCL/多壁奈米碳管（MWNTs）共混樣品。為了克服PCL與多壁奈米碳管間較差的相容性質，製備時選用丙烯酸接枝PCL（PCL-g-AA）和改質後含羥基多壁奈米碳管（MWNTs-OH）進行共混。比較PCL-g-AA /MWNTs-OH和PCL /MWNTs共混樣品間的差異時發現，前者的熱學和力學性質均優於後者； 舉例來說，僅添加5wt%的MWNTs-OH 就可大幅提升其初始熱分解溫度約77℃。 上述這種現象乃歸因於PCL-g-AA的羧酸基和MWNTs-OH的羥基反應形成酯基所致。最後發現最適化的MWNTs-OH添加量為5wt%，因為過多的MWNTs-OH，反而造成有機、無機的相分離而降低其相容性。

Three mixture systems of biodegradable polymers were prepared through melt blending processes in this thesis including poly(lactic acid) (PLA)/poly(vinyl alcohol) (PVA), PLA/poly(ε-caprolactone ) (PCL), and PCL/modified multi-walled carbon nanotubes (MWNTs). The properties of these mixtures investigated are including tensile propteies, thermal properties, crystallinity, microstructures, and optical properties.
In the first part, PLA and PVA were blended in various ratios by means of the melt blending method. The result of torque measurements and TGA tests showed that the addition of PLA can decrease the melt viscosity of PVA and that the second degradation step of PVA nearly disappeared for the PLA80PVA20 blend. The absorbance peaks of the carbonyl group and the hydroxyl group in the FTIR spectra of PLAxPVAy blends had significant shifts to lower wave numbers, indicating that there were interactions between these two groups. Combined with the result of DSC curves, this interaction would be favorable for improving miscibility. The XRD diffraction patterns and the PLM micrographs showed that PVA can serve as a nucleating agent to promote the crystallization of PLA in the PLAxPVAy blends. Moreover, the PLA80PVA20 blend gave the highest growth rate of PLA spherulite.
In the second part, a series of blends of PLA and PCL with different mass ratio were prepared by means of the melt blending method to study their crystallization, miscibility, morphology, and thermal and mechanical properties. The result of DSC tests showed that the melting temperatures of PLA and PCL shifted toward each other, and that the largest shift appeared at the PLA70PCL30 blend. This result reveals that the PLA70PCL30 blend gives the strongest interaction between these two polymers. The results of dynamic mechanical analysis and SEM morphologies show that PLA and PCL form a partial miscible blend, in which an amount of amorphous PCL is dissolved in the PLA-rich phase, leading to a depression of the Tg value. The polarized optical micrographs showed that PCL can serve as a nucleating agent to promote PLA crystallization in the PLAxPCLy blend. Moreover, the PLA70PCL30 blend gave the highest growth rate of PLA spherulite. Finally, the mechanical property of PLAxPCLy blends indicated that PLA can easily be tuned from rigid to ductile by the addition of PCL.
In the thord part, blends of PCL with MWNTs were prepared by means of a melt blending method. To cutail the poor compatibility between PCL and MWNTs, the acrylic acid grafted polycaprolactone (PCL-g-AA) and the multihydroxyl functionalized MWNTs (MWNTs-OH) were used as alternatives for the preparation of blends. As the comparison between PCL-g-AA/MWNTs-OH and PLA/MWNTs blends, the former gave much better thermal and mechanical properties than the latter; for example, the initial decomposition temperature was increased by 77°C with the addition of only 5wt%, owing to the formation of ester groups through the reaction between carboxyl groups of PCL-g-AA and hydroxyl groups of MWNTs-OH. Finally, the optimal amount of MWNTs-OH was 5wt% because excess MWNTs–OH caused separation of the organic and inorganic phases and lowering their
compatibility.

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