本研究以1,1,3,3-四甲基胍作為促進劑，使多元醇進行-胺基酸 N-羧酸酐開環聚合，成功地合成一系列三臂、四臂、六臂星狀聚胺基酸，去除保護基後加以改質，得到星狀聚賴胺酸-接枝-吲哚(PLL-g-Indo)、聚賴胺酸-接枝-苯環 (PLL-g-Phenyl)與聚穀胺酸-接枝-吲哚(PLG-g-Indo)，並將其製備成水膠。利用不同臂數目、聚合度及改質之疏水基團種類，探討不同分子型態與各種分子間作用力對水膠形成之影響，並以各種儀器分析水膠之微觀結構與機械性質。以各個接枝聚胺基酸進行成膠濃度測試，可以得知水合能力、靜電排斥力、π-π堆疊、氫鍵作用力、陽離子-π作用力對於水膠之形成扮演相當重要的角色，並且發現星狀結構可以明顯地增強分子間作用力，而同時增加臂的數目與聚合度可以有效地降低成膠濃度，其中六臂聚賴胺酸31-接枝-吲哚0.27(6-armed PLL31-g-Indo0.27)具有本研究中最低的臨界成膠濃度(0.75 wt%)。X光繞射圖譜證明PLL-g-Indo與PLL-g-Phenyl的疏水基團堆疊是形成水膠的原因之一，另外，由掃描式電子顯微鏡與小角度X光散射實驗發現星狀PLL-g-Indo水膠中，高分子堆疊成膜狀與部分纖維結構，並且可以得知臂數目的增加會使相關長度(mesh size)變小、聚合度的增加會使相關長度變大。進一步利用流變儀分析水膠的強度與回復情形，發現星狀PLL-g-Indo水膠之黏彈性質與臂的數目有關，並且回復能力極佳。由本研究的結果說明了星狀接枝聚賴胺酸水膠性質的可調控性，可以藉由改變臂數目、聚合度與改質之疏水基團種類控制水膠之微觀結構與機械性質。

In this study, we reported the synthesis and hydrogelation of linear and star-shaped graft poly(L-lysine) and poly(L-glutamic acid) (PLL-g-Indo, PLL-g-Phenyl and PLG-g-Indo). Star-shaped polypeptides were synthesized by N-carboxyanhydrides (NCAs) ring opening polymerization (ROP) using polyols as the initiators with the aid of 1,1,3,3-tetramethylguanidine (TMG), followed by deprotection and partial side chain modification. Successful synthesis of these polypeptides was confirmed by 1H NMR and GPC analyses. Investigation of circular dichroism (CD) spectroscopy suggested that PLL-g-Indo and PLL-g-Phenyl mainly adopted random coil conformation. PLL-g-Indo exhibited better gelation ability than PLL-g-Phenyl and PLG-g-Indo, which indicated that the balance between hydration, charge repulsion, π-π stacking, cation-π interaction and hydrogen bonding dictated the physically entangled gelation of polypeptides. In addition, compared to linear ones, the star-shaped architecture could efficiently promote intermolecular interactions between polypeptide chains. CGC decreased as arm number and arm length increased simultaneously, and 6-armed PLL31-g-Indo0.27 exhibited the lowest CGC of 0.75 wt%. XRD profiles showed that π-π stacking was one of the reasons to form hydrogel, while SAXS patterns could be described by the Ornstein-Zernike equation. Besides, SEM images revealed that polypeptide chains formed continuous, membranous hydrogel networks. Furthermore, rheological properties and mesh sizes of these star-shaped graft polypeptide hydrogels were found to depend on arm number, arm length and composition.

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