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Preparation and Characterization of Maleic Acid- Grafted Poly(butylene adipate-co-terephthalate)/ Layered Zinc Phenylphosphonate Nanocomposites
|關鍵字:||聚丁烯己二酸對苯二甲酸酯;層狀苯基磷酸鋅;奈米複合材料;結晶行為;生物降解特性;Poly(butylene adipate -co-terephthalate);Layered zinc phenylphosphonate;Nanocomposites;Crystalline behaviors;Microstructure;Biodegradable||引用:|| Y.-H. Na, Y. He, N. Asakawa, N. Yoshie, and Y. Inoue, 'Miscibility and Phase Structure of Blends of Poly(ethylene oxide) with Poly(3-hydroxybutyrate), Poly(3-hydroxypropionate), and Their Copolymers,' Macromolecules, vol. 35, no. 3, pp. 727-735, 2002.  N. Wu and H. Wang, 'Effect of zinc phenylphosphonate on the crystallization behavior of poly(l-lactide),' Journal of Applied Polymer Science, vol. 130, no. 4, pp. 2744-2752, 2013.  戈進杰, '生物高分子材料及其應用,' 2002, pp. 1-10.  日本生物可分解塑膠研究會, 圖解生物可分解塑膠.  R. A. Gross and B. Kalra, 'Biodegradable Polymers for the Environment,' Science, 10.1126/science.297.5582.803 vol. 297, no. 5582, p. 803, 2002.  G.-Q. Chen and M. K. 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聚丁烯己二酸對苯二甲酸酯（Poly（butylene adipate-co-terephthalate），PBAT）為環境友好之生物可分解高分子，擁有類似線性低密度聚乙烯的特性，非常具有發展潛力。本研究以不同莫耳比例之己二酸及對苯二甲酸二甲酯合成出PBAT，接著將馬來酸接枝於PBAT高分子鏈上，並利用化學插層法製備出有機改質PPZn，使PBAT高分子鏈插層進入有機改質PPZn層間時能有化學鍵結產生，以增強無機物與高分子基材的相容性，更進一步探討生物可分解高分子複合材料之結晶行為與不同形貌下的生物降解行為。使用XRD鑑定己烷二胺及十二烷基二胺改質PPZn的結構排列，層間距由原本的14.6 Å分別增加至24.1 Å與16 Å。由FT-IR圖譜觀察到改質後PPZn增加了波數為2853-3005 cm-1 和1650-1550 cm-1之吸收峰，表示長鏈烷基胺成功插層進入PPZn層間中，並經由溶劑插層法製備出不同比例之PBAT/C6-PPZn及C12-PPZn奈米複合材料，由XRD圖譜及TEM影像可以判斷改質PPZn以部分剝離與部分插層且隨機分散於PBAT 基材中，且添加改質PPZn並不會改變PBAT之結晶結構，再利用TGA分析複合材料熱穩定性，得知有機改質PPZn對於PBAT具有催化裂解效果。探討透過添加入不同比例C6-PPZn及C12-PPZn對於PBAT之等溫結晶行為影響，發現C6-PPZn之添加上升會使複合材料結晶速率提升，但當C12-PPZn添加比例越高時，結晶速率則是呈現由快至遲緩的趨勢。降解測試藉由假單胞菌（Lipase from Pseudomonas sp.）酵素酶作為降解液，再進行不同形貌之PBAT及其C6-PPZ和C12-PPZ奈米複合材料之生物降解測試，由其重量損失與降解時間之變化，可得知PBAT之降解速率會隨著馬來酸的加入及改質PPZn含量上升而使降解速率增加，且多孔形貌之重量損失程度相較於薄膜形貌更加顯著。
Poly(butylene adipate-co-terephthalate) (PBAT) is an environmentally friendly biodegradable polymer which contains the comparative physical properties to that of low-density polyethylene. In this study, PBAT was synthesized from different molar ratios of adipic acid and dimethyl terephthalate. Then, the maleic acid was grafted onto PBAT polymer chain (g-PBAT) and the organically modified PPZn was sucessfully synthesized to intercalate diaminohexane and dodecanediamine into the interlayer spacing of PPZn (designated as C6-PPZn and C12-PPZn) to improve the compatibility and dispersibility between the polymer and PPZn. Furthermore, the dispersion, crystallization and biodegradability of g-PBAT/organically modified PPZn nanocomposites were investigated systemtically.
The interlayer spacing of PPZn determined by wide-angle X-ray diffraction (WAXD) was increased from 14.6 Å for PPZn to 24.1 Å and 16 Å for C6-PPZn and C12-PPZn, respectively. Compared to the PPZn, the FT-IR spectra of organically modified PPZn contain absorption bands at 2853-3005 cm-1 and 1650-1550 cm-1 for the C-H stretching vibration and NH2 deformation from diaminohexane and dodecanediamine. The g-PBAT/ organically modified PPZn nanocomposites were prepared by solvent intercalation method. The structure and morphology of the g-PBAT/ organically modified PPZn nanocomposites were characterized by WAXD and transmission electron microscopy (TEM). The results of WAXD and TEM results show that the organically modified PPZn are randomly dispersed in the PBAT matrix. However, the addition of organically modified PPZn into PBAT would not change the crystalline structure of the nanocomposites. The results of isothermal crystallization show that the crystallization rate increases when the incorporation of C6-PPZn in nanocomposites increases, in contrast to C12-PPZn. Degradation tests was used Lipase from Pseudomonas sp. as the enzymatic degradation solution. Both the increasing content of organically modified PPZn and the presence of grafted maleic acid into PBAT would increase the weight loss of PBAT. In addition, the degradation rate of the porous morphology is more significant than the film morphology.
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