Phan Thi Ha My, Huang Ching-Chia, Tsai Yi-Jen, Hu Jin-Jia, Jan Jeng-Shiung
Department of Chemical Engineering, National Cheng Kung University, Tainan 70101, Taiwan.
Department of Mechanical Engineering, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan.
Gels. 2021 Aug 30;7(3):131. doi: 10.3390/gels7030131.
In this research, we studied the effect of polypeptide composition and topology on the hydrogelation of star-shaped block copolypeptides based on hydrophilic, coil poly(-lysine) (-PLL) tethered with a hydrophobic, sheet-like polypeptide segment, which is poly(-phenylalanine) (PPhe), poly(-leucine) (PLeu), poly(-valine) (PVal) or poly(-alanine) (PAla) with a degree of polymerization (DP) about 5. We found that the PPhe, PLeu, and PVal segments are good hydrogelators to promote hydrogelation. The hydrogelation and hydrogel mechanical properties depend on the arm number and hydrophobic polypeptide segment, which are dictated by the amphiphilic balance between polypeptide blocks and the hydrophobic interactions/hydrogen bonding exerted by the hydrophobic polypeptide segment. The star-shaped topology could facilitate their hydrogelation due to the branching chains serving as multiple interacting depots between hydrophobic polypeptide segments. The 6-armed diblock copolypeptides have better hydrogelation ability than 3-armed ones and -PLL--PPhe exhibits better hydrogelation ability than -PLL--PVal and -PLL--PLeu due to the additional cation-π and π-π interactions. This study highlights that polypeptide composition and topology could be additional parameters to manipulate polypeptide hydrogelation.
在本研究中，我们研究了多肽组成和拓扑结构对基于亲水性卷曲聚（赖氨酸）（-PLL）与疏水性片状多肽片段相连的星形嵌段共多肽水凝胶化的影响，该疏水性片状多肽片段为聚合度（DP）约为5的聚（苯丙氨酸）（PPhe）、聚（亮氨酸）（PLeu）、聚（缬氨酸）（PVal）或聚（丙氨酸）（PAla）。我们发现，PPhe、PLeu和PVal片段是促进水凝胶化的良好水凝胶剂。水凝胶化和水凝胶力学性能取决于臂数和疏水性多肽片段，这由多肽嵌段之间的两亲平衡以及疏水性多肽片段施加的疏水相互作用/氢键决定。星形拓扑结构由于支链作为疏水性多肽片段之间的多个相互作用位点，可促进它们的水凝胶化。六臂双嵌段共多肽比三臂共多肽具有更好的水凝胶化能力，并且由于额外的阳离子-π和π-π相互作用，-PLL--PPhe比-PLL--PVal和-PLL--PLeu表现出更好的水凝胶化能力。这项研究强调，多肽组成和拓扑结构可能是操纵多肽水凝胶化的额外参数。
