University of Rochester , Department of Chemistry, Rochester, New York 14627, United States.
Biomacromolecules. 2017 Nov 13;18(11):3591-3599. doi: 10.1021/acs.biomac.7b00925. Epub 2017 Sep 14.
Self-assembled peptide-based hydrogels are emerging materials that have been exploited for wound healing, drug delivery, tissue engineering, and other applications. In comparison to synthetic polymer hydrogels, supramolecular peptide-based gels have advantages in biocompatibility, biodegradability, and ease of synthesis and modification. Modification of the emergent viscoelasticity of peptide hydrogels in a stimulus responsive fashion is a longstanding goal in the development of next-generation materials. In an effort to selectively modulate hydrogel viscoelasticity, we report herein a method to enhance the elasticity of β-sheet peptide hydrogels using specific molecular recognition events between functionalized hydrogel fibrils and biomolecules. Two distinct biomolecular recognition strategies are demonstrated: oligonucleotide Watson-Crick duplex formation between peptide nucleic acid (PNA) modified fibrils with a bridging oligonucleotide and protein-ligand recognition between mannose modified fibrils with concanavalin A. These methods to modulate hydrogel elasticity should be broadly adaptable in the context of these materials to a wide variety of molecular recognition partners.
自组装肽基水凝胶是一种新兴材料，已被用于伤口愈合、药物输送、组织工程等应用。与合成聚合物水凝胶相比，基于超分子肽的水凝胶在生物相容性、可生物降解性以及易于合成和修饰方面具有优势。以响应性方式修饰肽水凝胶的突发粘弹性是开发下一代材料的长期目标。为了有选择性地调节水凝胶粘弹性，我们在此报告了一种使用功能化水凝胶原纤维与生物分子之间的特定分子识别事件来增强β-折叠肽水凝胶弹性的方法。展示了两种不同的生物分子识别策略：肽核酸（PNA）修饰原纤维与桥接寡核苷酸之间的寡核苷酸 Watson-Crick 双链体形成，以及甘露糖修饰原纤维与伴刀豆球蛋白 A 之间的蛋白-配体识别。这些调节水凝胶弹性的方法应该可以广泛适用于这些材料中的各种分子识别伴侣。
