本研究主旨是將生物可分解性高分子與不定型高分子或離子液體進行混摻，並觀察其結晶形貌與晶板排列。以聚羥基丁酸酯 [poly(hydroxybutyrate)，PHB]/對排聚甲基丙烯酸甲酯 [syndiotactic poly(methyl methacrylate)，sPMMA]與PHB/同排聚甲基丙烯酸甲酯 [isotactic poly(methyl methacrylate)，iPMMA]等混摻系統進行熱分析與相行為分析，發現兩個混摻系統存在相似的相行為，其上臨界溶液溫度(upper-critical-solution-temperature，UCST)分別約為225 oC以及240 oC。而在形貌觀察部分，sPMMA的對排性對球晶形貌的改變有著顯著的影響，相反地，iPMMA的同排性卻是幾乎沒有影響。在高含量sPMMA (如: 30 wt%)的PHB/sPMMA混摻系統中，在結晶溫度介於50-90 oC時，球晶均為負型(negative-birefringence)且無環帶狀(ringless)的球晶形貌。意味著本來neat PHB的環帶狀球晶受到干擾而完全消失，且PHB球晶的的光學特性也從本來的正型轉變成了負型球晶。但此現象並未發生在PHB/iPMMA混摻系統中。
在另外一個混摻系統聚丁二酸二乙酯[poly(ethylene succinate)，PESu]/聚對位乙烯基酚[poly(p-vinyl phenol)，PVPh]中，在不定型高分子含量為10-35 wt%、Tc = 40-70 oC且為超薄膜膜厚的條件下，可觀察到九種不同的結晶形貌。在單一的結晶溫度下，neat PESu從未被發現同時具有多樣的結晶形貌，但此狀況發生在PVPh含量大於20 wt%的PESu/PVPh混摻系統中。結晶溫度、膜厚/空間限制以及互有作用力存在的不定型PVPh的加入都是造成多樣球晶形貌的重要因素，部分原因來自PESu和PVPh間有很強的氫鍵作用力以及在擴散介面上有更好的成核能力。而在PESu/PVPh混摻體中，於膜厚約500 nm及熔融結晶溫度大於70 oC時所形成的PESu單晶形貌，利用AFM進行揭露。而TEM的電子繞射圖譜更進一步的證實PESu單晶的生成。薄的膜厚、較高的結晶溫度以及兩高分子間強作用力的存在，被認為是熔融結晶下形成PESu單晶的主要因素。
左式聚乳酸[poly(L-lactic)，PLLA]在特定的條件下可以發現到新穎的結晶形貌。低分子量的PLLA(LMw-PLLA)在熔融結晶溫度Tc = 110 oC時以及薄膜狀態下可觀察到六邊形的晶核，並從而發展出六邊形的環帶及出現在六個角的纖維稈狀結晶，球晶的最外圍則似有六片花瓣狀的球晶形貌。在環帶狀的形貌部分，可發現有序的寬和小的flat-on晶板，分離的排列形成具週期性高度變化的形貌，然而在纖維狀區域則發現晶板以連續的flat-on，微傾及edge-on方式進行排列。初始的幾何形狀被認為是影響最終球晶形貌的重要因素。
在左式聚乳酸[poly(L-lactic)，PLLA]混摻離子液體[ionic liquid，IL]系統中， LMw-PLLA因IL的添加而出現多樣的球晶形貌，且並未在neat PLLA中被觀察到。在具甘氨酸酯基的離子液體摻合下，首次發現具有星形晶核的PLLA新型六角形結晶形貌。離子液體的塑化效果導致球晶成長初期具有較快的成核和生長速率。而在球晶成長的後期，離子液體的含量提高讓高分子鏈的流動性更為增加，使得結晶形貌從六邊形轉變為星形的球晶形貌。另外在PLLA/IL的混摻系統中，當離子液體的含量較高時也可以觀察到特殊的枝狀結晶形貌。隨著離子液體的含量增加，PLLA球晶成長速率變慢且PLLA的玻璃轉換溫度(Tg)下降，這都說明了離子液體PLLA所造成的塑化作用以及兩者間存在的作用力阻礙了PLLA的熔融結晶。PLLA在結晶後的冷卻過程中，常展現材料脆性且有大規模的裂縫生成，然而在加入離子液體後，會使裂縫的形成減少甚至消失。

This study has been focused on the crystalline morphology and lamellar arrangement of biodegradable polymers blended with amorphous polymers or ionic liquid. Blends of poly(hydroxybutyrate)/syndiotactic poly(methyl methacrylate) (PHB/sPMMA) and poly(hydroxybutyrate)/isotactic poly(methyl methacrylate) (PHB/iPMMA) exhibited similar phase behavior which is upper-critical-solution-temperature (UCST) at ~225 oC and ~240 oC respectively, based on the results of thermal analysis and phase morphology. However, syndiotacticity in PMMA exerts a prominent effect on altering the PHB spherulites morphology while, by contrast, isotacticity in PMMA has most no effect at all. At high sPMMA contents (e.g., 30 wt%) in the PHB/sPMMA blend, the spherulites are all negative-birefringence and ring-less when crystallized at any crystallization temperature (Tc) between 50-90 oC. That is, not only the original ring-banded pattern in neat PHB spherulites is completely disrupted, but the optical sign is reverted completely from positive- to negative-birefringence in sPMMA/PHB blend, but not seen in isotactic PMMA/PHB one.
A total of nine different types of crystalline morphology were identified in the poly(ethylene succinate)/poly(p-vinyl phenol) (PESu/PVPh) blend with amorphous contents from 10 to 35 wt% and Tc = 40-70 oC in ultra-thin film thickness. Multiple types of PESu crystalline morphology at the same Tc are never seen in neat PESu, but occur in PESu/PVPh blend with amorphous PVPh higher than 20 wt%. Crystallization temperature, thickness/space confinement, and presence of interacting amorphous PVPh are the main factors for multiple types of spherulites in the blends, partly due to strong interactions via hydrogen bonding between PESu and PVPh and likely extra nucleation capacity from the diffusion interfaces. Single crystals of PESu were proven by AFM in the PESu/PVPh blend especially when confined in films of around 500 nm, melt-crystallized at Tc =70 oC or above. The electron diffraction pattern of TEM result further confirmed the formation of PESu single crystals. The combination of thin film thickness, high crystallization temperature, and strong interaction between two polymers were believed as the main factors for melt-crystallized PESu single crystals.
Novel morphology is found in neat PLLA at specific condition. The six-petal spherulite morphology composed of a combination of a central hexagon core, hexagon-shape ring bands and fibrous six stalks was discovered in a low molecular weight PLLA (LMw-PLLA) melt-crystallized at a specific Tc =110oC and confined in thin films. Discrete lamellae, consisting of sequenced wide and small lamellae, all in flat-on orientation with periodically up-and-down topology, were packed in ring-banded alignment, while continuous lamellae in flat-on, tilted, or edge-on orientation were arranged in fibrous region. The geometry of the initial crystal was believed to be the influencing factors in final spherulite patterns. Crystalline morphology of poly(L-lactide) (PLLA) is significantly changed by the addition of ionic liquid (IL) to display a diversification of spherulites morphology which never been seen before in neat PLLA. A hexagonal crystal with star-shaped core, a novel crystal morphology never seen before, in LMw-PLLA modified by glycine ester based ionic liquid. The plasticizing effect of the ionic liquid leads to faster nucleation and growth rate in the early stage of crystallization. In the latter stage of crystal growth, the increase in polymer chain mobility, enhanced by the ionic liquid addition, leads to a morphology transformation from hexagon-shape to star-shape morphology. Special dendritic morphology is also observed in PLLA/IL blend with higher IL content. The existence of the IL-PLLA interaction impedes the melt crystallization of PLLA, indicated by the decrease in spherulitic growth rate with increasing IL content, and the glass transition (Tg) of PLLA decreases with the increase in IL content, showing the plasticizing effect to PLLA. Neat PLLA shows brittleness with extensive crack formation during post-crystallization cooling process; however, after the addition of IL, the crack formation is reduced or even diminished.

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