本實驗利用偏光顯微鏡 (polarized-light optical microscopy，POM)、微分掃描熱卡計 (differential scanning calorimetry，DSC)、傅立葉轉換紅外線光譜儀 (Fourier-transfer infrared spectrometer，FTIR)、廣角X光繞射儀 (wide-angle X-ray diffraction，WAXD)、原子力電子顯微鏡 (atomic-force microscopy，AFM)、環境式掃描電子顯微鏡 (environmental scanning electron microscopy，ESEM) 以及小角度X光散射儀 (small angle X-ray scattering，SAXS) 來探討聚羥基丁酸酯 [poly(3-hydroxybutyrate)，PHB]與聚丙烯酸甲酯 [poly(methyl acrylate)，PMA] 混摻系統的球晶型態正負型及其馬爾它十字旋轉的行為。

研究中發現，PHB會因為PMA的添加 (≧30 wt%) 造成球晶型態隨結晶溫度的升高而從負型的馬爾它十字球晶 (Tc= 55～60 oC) 順時針旋轉至正型的馬爾它十字球晶 (Tc= 70～90 oC)。針對可能的影響因素進行討論發現，影響最大的因素為與PHB混摻的不定型高分子種類以及混摻比例，而PHB的分子量、樣品膜厚、熔融溫度及熔融時間僅對其旋轉發生的結晶溫度範圍造成些微影響。結晶溫度的上升會伴隨著PMA部分鏈段逐漸陷入PHB晶板之中 (interlamellar區域)，導致PMA鏈段在intraspherulite區域形成球狀顆粒domain的數量減少，也使得PHB的晶體變得較不完美，而在DSC的升溫曲線圖中觀察到較明顯的shoulder peak。FTIR及WAXD分析則發現，馬爾它十字出現旋轉的原因並非來自分子間作用力及晶格改變所造成。SEM及AFM的觀察結果，推測PMA在球晶內部所形成的球狀amorphous顆粒，影響了PHB晶板的傾斜方向，即當結晶溫度較低時，PMA於樣品中以顆粒小且數量多的球狀domain方式存在，大大地限制了PHB的晶板成長方向，使晶板被迫以edge-on或些微傾斜的edge-on方式進行排列，而當結晶溫度升高，PMA所組成的球狀顆粒有較久的時間聚集，使得尺寸變大數量下降，部分PMA的鏈段亦開始陷入PHB的晶板之間，PHB晶板的排列方式回到原本neat PHB具有的正型馬爾它十字球晶。相較於常見的片狀或是連續的帶狀相分離domain，本實驗發現當樣品中的不定型高分子以球狀顆粒的方式存在，也將對高分子球晶內部晶板的方向造成影響，進而影響其光學上的球晶型態。

In this study, the crystal morphology and the birefringence of poly(3-hydroxybutyrate)/poly(methyl acrylate) (PHB/PMA) blends were studied by using polarized-light optical microscopy (POM), differential scanning calorimetry (DSC), Fourier-transfer infrared spectrometer (FTIR), wide-angle X-ray diffraction (WAXD), atomic-force microscopy (AFM), environmental scanning electron microscopy (ESEM) and small angle X-ray scattering (SAXS).

PHB/PMA blends with PMA content more than 30 wt%, the Maltese cross of the spherulite rotate clockwise from negative- to positive-type spherulite with increasing Tc. The properties of amorphous polymers and the blend composition were the most important factors for the Maltese cross rotation phenomenon rather than the molecular weight of PHB, sample thickness, melting temperature, and melting time. At higher Tc, the DSC results show multiple melting peaks due to the melt of imperfect crystals. Moreover, the SEM results show that the number of PMA domains in the intraspherulite regions of PHB spherulites is reduced with increasing Tc. These two results indicate that some PMA molecular chains might be trapped into the interlamellar regions of PHB crystals, leading to the formation of imperfect PHB crystals. From FT-IR and WAXD results, the rotation phenomenon from negative- to positive-type spherulite was not caused by molecular interactions or crystal form difference. The mechanism of the rotation phenomenon of the Maltese cross in this blends is supposed to be the tilt of PHB lamellae from edge-on at lower Tc (induced by numerous tiny spherical PMA domains) to flat-on lamellae with a little tilt forward or backward to the nucleus at higher Tc. Interestingly, these spherical amorphous domains are considered to be able to influence the lamellar orientation and the optical birefringence.

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