Molecular design for growth of supramolecular membranes with hierarchical structure

R. Helen Zha, Yuri S. Velichko, Ronit Bitton, Samuel I Stupp

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

Membranes with hierarchical structure exist in biological systems, and bio-inspired building blocks have been used to grow synthetic analogues in the laboratory through self-assembly. The formation of these synthetic membranes is initiated at the interface of two aqueous solutions, one containing cationic peptide amphiphiles (PA) and the other containing the anionic biopolymer hyaluronic acid (HA). The membrane growth process starts within milliseconds of interface formation and continues over much longer timescales to generate robust membranes with supramolecular PA-HA nanofibers oriented orthogonal to the interface. Computer simulation indicates that formation of these hierarchically structured membranes requires strong interactions between molecular components at early time points in order to generate a diffusion barrier between both solutions. Experimental studies using structurally designed PAs confirm simulation results by showing that only PAs with high ζ potential are able to yield hierarchically structured membranes. Furthermore, the chemical structure of such PAs must incorporate residues that form β-sheets, which facilitates self-assembly of long nanofibers. In contrast, PAs that form low aspect ratio nanostructures interact weakly with HA and yield membranes that exhibit non-fibrous fingering protrusions. Furthermore, experimental results show that increasing HA molecular weight decreases the growth rate of orthogonal nanofibers. This result is supported by simulation results suggesting that the thickness of the interfacial contact layer generated immediately after initiation of self-assembly increases with polymer molecular weight.

Original languageEnglish
Pages (from-to)1401-1410
Number of pages10
JournalSoft Matter
Volume12
Issue number5
DOIs
Publication statusPublished - 2016

Fingerprint

membranes
Membranes
Hyaluronic Acid
Nanofibers
Self assembly
self assembly
Amphiphiles
acids
peptides
molecular weight
Molecular weight
low aspect ratio
Peptides
Biopolymers
Diffusion barriers
Molecular interactions
biopolymers
Biological systems
Interfaces (computer)
Aspect ratio

ASJC Scopus subject areas

  • Chemistry(all)
  • Condensed Matter Physics

Cite this

Molecular design for growth of supramolecular membranes with hierarchical structure. / Helen Zha, R.; Velichko, Yuri S.; Bitton, Ronit; Stupp, Samuel I.

In: Soft Matter, Vol. 12, No. 5, 2016, p. 1401-1410.

Research output: Contribution to journalArticle

Helen Zha, R. ; Velichko, Yuri S. ; Bitton, Ronit ; Stupp, Samuel I. / Molecular design for growth of supramolecular membranes with hierarchical structure. In: Soft Matter. 2016 ; Vol. 12, No. 5. pp. 1401-1410.
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