Biomimetic assemblies using peptides for the formation of designed nanostructures exhibit several attractive features for biotechnological applications. Peptides are computationally designed to self-assemble into coiled coil bundles that serve as building blocks, or “bundlemers” for the construction of higher order materials. The bundlemers are homotetrameric coiled coils with an antiparallel arrangement of the constituent helices, giving rise to two N-termini and C-termini at each end of the bundlemers. The complementary bundlemers whose N-termini at both ends are functionalized with either maleimide or thiol are conjugated with each other via a thiol-Michael reaction to construct bundlemer chains. By managing the stoichiometries of the functionalized bundlemers and the covalent interactions in the chain formation, the length of the bundlemer chains is desirably controlled. The bundlemer chains display extreme axial rigidity due to the bundlemer rigidity and the direct covalent attachment between bundlemers. The rigid rod character of the bundlemer chains produces lyotropic liquid crystalline behavior in concentrated solution, which is effective in the preparation of oriented nanostructures. The unidirectional orientation of the bundlemer chains in aqueous solution is determined optically by birefringence observation and rheological behavior at various concentrations. In addition, the bundlemer chains are used to fabricate continuous nanofibers, preserving their unique orientational behavior within the fibers. The uniform nanofibers are constructed from the concentrated solution of the bundlemer chains by using the electrospinning technique which produces fibers with excellent molecular alignment. The rigid bundlemer chains are aligned along the fiber axis due to the solution liquid crystallinity and elongational flow during the electrospinning process. The inner orientational order of the bundlemer chains in the electrospun nanofibers is observed in thin cross sections of the electrospun nanofibers via electron microscopy as well as spectroscopy. Mechanical properties of the peptide bundlemer rod fibers also will be presented.

Molecular interactions and orientation of rigid bundlemer rod chains in electrospun nanofibers

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.