Hydrogels have been widely explored for use as materials in assorted biomedical applications, including as tissue engineering scaffolds, antifouling surfaces, and drug delivery vehicles. A number of peptides have been reported to self-assemble into robust hydrogels via inter-strand crosslinking. However, peptide-based materials pose practical and clinical challenges as a result of their susceptibility to proteolytic degradation and the relative difficulty associated with chemical functionalization of their side chains. <b>Here, we study the influence of polymer architecture on hydrogel assembly and viscoelastic properties from a series of biosynthetic polymer mimics of the KLD-12 peptide, which is known to form hydrogels by a combination of electrostatic and hydrophobic interactions.</b> In our design, analogues of the comprising amino acids are prepared as modified norbornene monomers and polymerized by ring opening metathesis polymerization (ROMP). With this strategy, the peptide backbone is replaced with a norbornene backbone that is resistant to proteolytic degradation and can be easily modified to include a wide range of chemical functionality. The architectural influence of block vs random copolymers, degree of polymerization, block size, and hydrophobic content, were studied; rheological characterization of these materials elucidated their impact on hydrogel stiffness (G’), elasticity (G”), swelling, healing potential, viscous shearing, and temperature sensitivity. This comparison between the physical properties of our polymer mimics to those of the parent peptide demonstrate the utility and versatility in design of self-assembling proteolytic resistant biosynthetic polymer hydrogels. <b>Critically, simple architectural modifications during polymerization may allow access to a variety of materials suited to different biomedical applications</b>.

Architectural influence on the assembly of biosynthetic polymer analogues to a peptide hydrogel

253rd National Meeting (2017)

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