本研究主要針對聚左旋乳酸(Poly L-lactic acid, PLLA)和聚右旋乳酸(Poly D-lactic acid, PDLA)共混後聚合物和纖維的均聚物和立構複合物的結晶行為，分為四章節討論。各章節討論的主題分別為，第三章：聚乳酸立構複合結晶行為與球晶型態、第四章: PLLA/PDLA (LD)共混纖維於升溫過程中均聚物和立構複合物的結晶行為、第五章：PLLA/PDLA/PHBV共混纖維的製備與結晶行為、和第六章：不同儲存條件下PLLA/PDLA共混聚合體的熱穩定性和結晶行為。
第三章依據Lauritzen-Hoffman二次成核理論，探討立構複合物結晶的regime II→III轉移溫度。發現立構複合物結晶的regime II→III轉移溫度在165 °C，不會因為共混比例的不同而改變。利用兩步等溫結晶條件形成立構複合物結晶和均聚物結晶所組成的同心圓球晶，在同心圓內受限空間的球晶生長速率和未受限空間生長的球晶生長速率有所不同。第四章探討PLA纖維於升溫過程中分子鏈的熱鬆弛現象，均聚物和立構複合物冷結晶、熔融、與再結晶行為；發現通過紡絲過程，將會導致分子鏈更近一步一對一排列，從而促進立構複合物結晶再升溫過程中的形成。第五章針對少量PHBV加入PLA對其結晶行為的探討，發現少量PHBV加入PLA打亂PLA分子鏈的規整性，導致共混聚合體的PLA結晶程度隨著PHBV含量的增加而降低；如在PLLA/PDLA/PHBV條件下，立構複合物結晶的產生可以改善均聚物的結晶行為；共混纖維中並沒有觀察到立構複合物結晶的存在。第六章探討PLLA、PDLA、和LD於室溫儲存在真空袋和在乾燥箱內三年後的熱穩定性和結晶行為，發現儲存在真空袋和在乾燥箱內材料的水解行為明顯不同；存放在乾燥箱內有明顯的水解行為發生，導致其熱穩定性明顯下降、熔點下降和熱焓上升。存放在乾燥箱的LD-D只有立構複合物結晶產生，沒有均聚物結晶存在。

The focus of this research is the homocrystallization and stereocomplex crystallization in poly(L-lactide)/poly(D-lactide) blends and fibers. This study is divided into four chapters: Chapter 3. Crystallization and spherulite morphology of polylactide stereocomplex; Chapter 4. Homocrystallization and stereocomplex crystallization behaviors of as-spun and hot-drawn PLLA/PDLA blended fibers during heating; Chapter 5. Formation and fiber structure of PLLA/PDLA/PHBV blended fibers; Chapter 6. Effect of storage conditions on the thermal stability and crystallization behaviors of PLLA/PDLA.
In Chapter 3, it was found that the regime II → III transition temperature of stereocomplex crystals in the Lauritzen–Hoffman plot of the LD blends was determined to be 165 °C. A concentric spherulite consisting of stereocomplex crystals and homocrystals formed under two-step isothermal crystallisation conditions with three growth stages was observed. The confined spherulitic growth rate in the concentric spherulite and the unrestricted spherulitic growth rate in individual spherulite were also analysed. In Chapter 4, we studied the movement of fiber molecular chains, including the orientation and relaxation of molecular chains, as well as crystallization, melting, and recrystallization of homocrystals and stereocomplex crystals. The side-by-side packing of the molecular chains was promoted by mixing the molecular chains with the extrusion screw during the spinning process, facilitating stereocomplex crystallization. In Chapter 5, it was found that the addition of PHBV to PLLA would disrupt the regularity of the PLA molecular chains, resulting in a decrease in the crystallinity of PLA of PLLA/PHBV blends, but the formation of stereocomplex crystal may be beneficial to the crystallization of PLLA/PDLA/PHBV blends. No stereocomplex crystal were observed in PLLA/PDLA/PHBV fibers. In Chapter 6, the differences in the hydrolysis of PLLA, PDLA, and LD samples under two sets of laboratory storage conditions for 3 years were studied. When stored in vacuum-sealed bags, PLLA, PDLA, and LD samples hydrolyzed slowly; while when stored in a vacuum-free desiccator, they degraded significantly. This process significantly reduced the thermal stability of the samples stored in the vacuum-free desiccator, resulting in a lower melting point and an increase in the endothermic enthalpy. When the LD sample was stored in a vacuum-free desiccator, only stereocomplex crystals were formed, and no homocrystals were observed.

誌謝 I
摘要 II
ABSTRACT IV
目 錄 VI
第1章 緒論 1
1.1簡介 1
1.2聚乳酸 3
1.3聚乳酸立構複合物結晶 5
1.4研究目的 10
第2章 實驗儀器與分析技術 11
2.1廣角X光繞射儀(WIDE ANGLE X-RAY DIFFRACTION, WAXD) 11
2.2同步輻射廣角X光散射儀(SYNCHROTRON WIDE ANGLE X-RAY DIFFRACTION, WAXD) 11
2.3調製溫度式微差掃描熱分析儀(MODULATED DIFFERENTIAL SCANNING CALORIMETER, MDSC) 12
2.4可加熱式偏光顯微鏡(HOT STAGE POLARIZING MICROSCOPE, HSPM) 14
2.5熱重分析儀(THERMALGRAVIMETRIC ANALYZER, TGA) 16
2.6凝膠滲透層析儀(GEL PERMEATION CHROMATOGRAPHY, GPC) 17
2.7纖維順向度量測儀(ACOUSTIC INSTRUMENT) 17
第3章 聚乳酸立構複合結晶行為與球晶型態 19
3.1 DSC分析 20
3.1.1試樣準備與實驗 20
3.1.2 結晶與熔融行為分析 21
3.1.2非等溫結晶動力學分析 25
3.3 WAXD分析 28
3.3.1試樣準備與實驗 28
3.3.2結晶結構分析 28
3.5 二次成核動力學分析 31
3.5.1 試樣準備與實驗 31
3.5.2 regime轉移分析 32
3.5.2 球晶形態分析 35
3.4 同心圓球晶分析 36
3.4.1 試樣準備與實驗 36
3.4.1 立構複合物結晶與均聚物結晶組成同心圓 36
3.5 小結 42
第4章 PLLA/PDLA共混纖維於升溫過程中均聚物和立構複合物的結晶行為 45
4.1 結晶結構與順向分析 47
4.1.1試樣準備與實驗 47
4.1.2 LD共混切粒晶體結構與順向分析 48
4.1.3 LD共混纖維晶體結構與順向分析 49
4.2熱性質分析 52
4.2.1試樣準備與實驗 52
4.3.2 標準DSC結晶與熔融行為分析 53
3.3.3 調制溫度式DSC結晶與熔融行為分析 56
4.3升溫過程中的結晶變化分析 59
4.3.1試樣準備與實驗 59
4.3.2 HSPM升溫觀察 59
4.3.3 Real-time WAXD升溫觀察 63
4.4 小結 65
第5章 PLLA/PDLA/PHBV共混纖維的製備與結晶行為探討 67
5.1 DSC分析 69
5.1.1試樣準備與實驗 69
5.1.2 結晶與熔融行為分析 70
5.2 WAXD晶體結構分析 75
5.2.1試樣準備與實驗 75
5.2.2 LH和LDH共混切粒晶體結構分析 75
5.2.3 LH和LDH共混纖維晶體結構分析 79
5.3 纖維順向度分析 80
5.3.1試樣準備與實驗 80
5.3.2分子鏈順向分析 81
5.3.3結晶順向度分析 83
5.4 小結 84
第6章 不同儲存條件下PLLA/PDLA共混聚合體的熱穩定性和結晶行為 87
6.1 TGA分析 90
6.1.1試樣準備與實驗 90
6.1.2非等溫熱裂解行為 90
6.2 GPC分析 92
6.2.1試樣準備與實驗 92
6.2.2分子量分佈 92
6.3 DSC分析 94
6.3.1試樣準備與實驗 94
6.1.2 結晶與熔融行為分析 95
6.4 WAXD分析 98
6.4.1試樣準備與實驗 98
6.4.2熔融前與熔融後結晶結構變化 99
6.5 小結 101
第7章 結論 103
參考文獻 106

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