Isomeric control of the mechanical properties of supramolecular filament hydrogels

Yi An Lin, Myungshim Kang, Wei Chiang Chen, Yu Chuan Ou, Andrew G. Cheetham, Pei Hsun Wu, Denis Wirtz, Sharon M. Loverde, Honggang Cui

Research output: Contribution to journalArticle

Abstract

Supramolecular filament hydrogels are an emerging class of biomaterials that hold great promise for regenerative medicine, tissue engineering, and drug delivery. However, fine-tuning of their bulk mechanical properties at the molecular level without altering their network structures remains a significant challenge. Here we report an isomeric strategy to construct amphiphilic peptides through the conjugation of isomeric hydrocarbons to influence the local viscoelastic properties of their resulting supramolecular hydrogels. In this case, the packing requirements of the chosen isomeric hydrocarbons within the supramolecular filaments are dictated by their atomic arrangements at the molecular and intermolecular levels. Atomistic molecular dynamics simulations suggest that this design strategy can subtly alter the molecular packing at the interface between the peptide domain and the hydrophobic core of the supramolecular assemblies, without changing both the filament width and morphology. Our results from wide-angle X-ray scattering and molecular simulations further confirm that alterations to the intermolecular packing at the interface impact the strength and degree of hydrogen bonding within the peptide domains. This subtle difference in the isomeric hydrocarbon design and their consequent packing difference led to variations in the persistence length of the individual supramolecular filaments. Microrheological analysis reveals that this difference in filament stiffness enables the fine-tuning of the mechanical properties of the hydrogel at the macroscopic scale. We believe that this isomeric platform provides an innovative method to tune the local viscoelastic properties of supramolecular polymeric hydrogels without necessarily altering their network structures.

Original languageEnglish (US)
Pages (from-to)216-224
Number of pages9
JournalBiomaterials Science
Volume6
Issue number1
DOIs
StatePublished - Jan 1 2018

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Hydrogels
Hydrocarbons
Peptides
Mechanical properties
Tuning
Hydrogel
Biocompatible Materials
X ray scattering
Drug delivery
Tissue engineering
Biomaterials
Molecular dynamics
Hydrogen bonds
Stiffness
Computer simulation

ASJC Scopus subject areas

  • Biomedical Engineering
  • Materials Science(all)

Cite this

Lin, Y. A., Kang, M., Chen, W. C., Ou, Y. C., Cheetham, A. G., Wu, P. H., ... Cui, H. (2018). Isomeric control of the mechanical properties of supramolecular filament hydrogels. Biomaterials Science, 6(1), 216-224. https://doi.org/10.1039/c7bm00722a

Isomeric control of the mechanical properties of supramolecular filament hydrogels. / Lin, Yi An; Kang, Myungshim; Chen, Wei Chiang; Ou, Yu Chuan; Cheetham, Andrew G.; Wu, Pei Hsun; Wirtz, Denis; Loverde, Sharon M.; Cui, Honggang.

In: Biomaterials Science, Vol. 6, No. 1, 01.01.2018, p. 216-224.

Research output: Contribution to journalArticle

Lin, YA, Kang, M, Chen, WC, Ou, YC, Cheetham, AG, Wu, PH, Wirtz, D, Loverde, SM & Cui, H 2018, 'Isomeric control of the mechanical properties of supramolecular filament hydrogels', Biomaterials Science, vol. 6, no. 1, pp. 216-224. https://doi.org/10.1039/c7bm00722a
Lin, Yi An ; Kang, Myungshim ; Chen, Wei Chiang ; Ou, Yu Chuan ; Cheetham, Andrew G. ; Wu, Pei Hsun ; Wirtz, Denis ; Loverde, Sharon M. ; Cui, Honggang. / Isomeric control of the mechanical properties of supramolecular filament hydrogels. In: Biomaterials Science. 2018 ; Vol. 6, No. 1. pp. 216-224.
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