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Engineering bio-inspired peptide-polyurea hybrids with thermo-responsive shape memory behaviour.

Daseul Jang1, Chase B Thompson1, Sourav Chatterjee1

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Peptide secondary structures in polymer hybrids tune thermo-responsive shape memory. Beta-sheet motifs decrease shape fixity, while alpha-helical structures enhance it by controlling hydrogen bonding and phase mixing.

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Biomaterials

Background:

  • Nature's tunable materials inspire synthetic approaches.
  • Controlling hierarchical structure is key to advanced material properties.
  • Peptide motifs offer a route to tailor polymer characteristics.

Purpose of the Study:

  • To investigate how peptide secondary structures influence hierarchical ordering and thermo-responsive shape memory in peptide-polymer hybrids.
  • To explore the role of hydrogen bonding in modulating shape memory behavior.
  • To demonstrate temperature-induced shifts in secondary structure for tunable responses.

Main Methods:

  • Synthesis of poly(β-benzyl-L-aspartate)-b-poly(dimethylsiloxane)-b-poly(β-benzyl-L-aspartate) based peptide-polyurea hybrids.
  • Characterization using attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR), small-angle X-ray scattering (SAXS), and dynamic mechanical analysis (DMA).
  • Analysis of microphase-separated morphology, shape fixity, and shape recovery.

Main Results:

  • Beta-sheet motifs promoted phase mixing and decreased shape fixity due to extensive inter-molecular hydrogen bonding.
  • Alpha-helical arrangements led to microphase separation, hierarchical ordering, and increased shape fixity via intra-molecular hydrogen bonding.
  • Temperature-dependent shifts in peptide secondary structure were shown to influence shape memory response.

Conclusions:

  • Peptide secondary conformation is a critical factor in tuning the hierarchical structure and shape memory properties of peptide-polymer hybrids.
  • Hydrogen bonding character and phase mixing between peptide and polymer segments dictate shape memory behavior.
  • This research enables the design of smart, bio-inspired materials with tailored, responsive functions.