Molecular Design: Network Architecture and Its Impact on the Organization and Mechanics of Peptide-Polyurea Hybrids

Lindsay Matolyak, Jong Keum, La Shanda T.J. Korley

Research output: Contribution to journalArticlepeer-review

16 Scopus citations

Abstract

Nature has achieved controlled and tunable mechanics via hierarchical organization driven by physical and covalent interactions. Polymer-peptide hybrids have been designed to mimic natural materials utilizing these architectural strategies, obtaining diverse mechanical properties, stimuli responsiveness, and bioactivity. Here, utilizing a molecular design pathway, peptide-polyurea hybrid networks were synthesized to investigate the role of architecture and structural interplay on peptide hydrogen bonding, assembly, and mechanics. Networks formed from poly(β-benzyl-l-aspartate)-poly(dimethylsiloxane) copolymers covalently cross-linked with a triisocyanate yielded polyurea films with a globular-like morphology and parallel β-sheet secondary structures. The geometrical constraints imposed by the network led to an increase in peptide loading and ∼7x increase in Young’s modulus while maintaining extensibility (∼160%). Thus, the interplay of physical and chemical bonds allowed for the modulation of resulting mechanical properties. This investigation provides a framework for the utilization of structural interplay and mechanical tuning in polymer-peptide hybrids, which offers a pathway for the design of future hybrid biomaterial systems.

Original languageEnglish
Pages (from-to)3931-3939
Number of pages9
JournalBiomacromolecules
Volume17
Issue number12
DOIs
StatePublished - Dec 12 2016

Funding

The authors acknowledge funding support from the National Science Foundation (CAREER DMR-0953236). The authors thank Richard Tomazin from the Swagelok Center for Surface Analysis of Materials at Case Western Reserve University for AFM image assistance on all film samples.

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