Responsive hydrogels from the intramolecular folding and self-assembly of a designed peptide
Responsive hydrogels from the intramolecular folding and self-assembly of a designed peptide
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DOI：
10.1021/ja027993g
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发表时间：
2002-12-18
影响因子：
15
通讯作者：
Kretsinger, J
中科院分区：
文献类型：
--
作者：
Schneider, JP;Pochan, DJ;Kretsinger, J
一个一般的肽设计，链接的pH值依赖性的分子内折叠的P-发夹肽的倾向，自组装，提供水凝胶富含β-片。化学响应性已经通过将分子内折叠与溶液pH值的变化联系起来而被专门设计到材料中，并且机械响应性通过将水凝胶化与自组装联系起来而被专门设计到材料中。圆二色性和红外光谱表明，在低pH值下，单个肽是非结构化的，从而提供低粘度的水溶液。在碱性条件下，分子内折叠发生，提供分子间自组装的两亲性β-发夹。流变学表明，所得水凝胶是刚性的，但剪切稀化。然而，由于支架固有的自组装性质，观察到剪切停止后的快速机械强度恢复。凝胶化过程的表征，从分子水平到材料的宏观性质，表明通过将小的设计肽的分子内折叠与它们的自组装能力联系起来，可以制备响应性材料。低温透射电子显微镜和激光扫描共聚焦显微镜揭示了纳米和微米尺度上的水填充的多孔支架。环境响应性、形态学和肽性质使这种水凝胶成为生物医学和工程技术的可能材料候选者。
A general peptide design is presented that links the pH-dependent intramolecular folding of P-hairpin peptides to their propensity to self-assemble, affording hydrogels rich in beta-sheet. Chemical responsiveness has been specifically engineered into the material by linking intramolecular folding to changes in solution pH, and mechanical responsiveness, by linking hydrogelation to self-assembly. Circular dichroic and infrared spectroscopies show that at low pH individual peptides are unstructured, affording a low-viscosity aqueous solution. Under basic conditions, intramolecular folding takes place, affording amphiphilic beta-hairpins that intermolecularly self-assemble. Rheology shows that the resulting hydrogel is rigid but is shear-thinning. However, quick mechanical strength recovery after cessation of shear is observed due to the inherent self-assembled nature of the scaffold. Characterization of the gelation process, from the molecular level up through the macroscopic properties of the material, suggests that by linking the intramolecular folding of small designed peptides to their ability to self-assemble, responsive materials can be prepared. Cryo-transmission electron and laser scanning confocal microscopies reveal a water-filled porous scaffold on both the nano- and microscale. The environmental responsiveness, morphology, and peptidic nature make this hydrogel a possible material candidate for biomedical and engineering technology.