Supramolecular Self-Assembly To Control Structural and Biological Properties of Multicomponent Hydrogels

Babatunde O Okesola; Yuanhao Wu; Burak Derkus; Samar Gani; Dongsheng Wu; Dafna Knani; David K Smith; Dave J Adams; Alvaro Mata

doi:10.1021/acs.chemmater.9b01882

Supramolecular Self-Assembly To Control Structural and Biological Properties of Multicomponent Hydrogels

Chem Mater. 2019 Oct 8;31(19):7883-7897. doi: 10.1021/acs.chemmater.9b01882. Epub 2019 Sep 12.

Authors

Babatunde O Okesola^{1

2}, Yuanhao Wu^{1

2}, Burak Derkus^{1

2

3}, Samar Gani⁴, Dongsheng Wu², Dafna Knani⁴, David K Smith⁵, Dave J Adams⁶, Alvaro Mata^{1

2}

Affiliations

¹ Institute of Bioengineering, Queen Mary University of London, London E1 4NS, U.K.
² School of Engineering and Materials Science, Queen Mary University of London, London E1 4NS, U.K.
³ Biomedical Engineering Department, Faculty of Engineering, Eskisehir Osmangazi University, 26040 Eskisehir, Turkey.
⁴ Department of Biotechnology Engineering, ORT Braude College, P.O. Box 78, Karmiel 2161002, Israel.
⁵ Department of Chemistry, University of York, Heslington, York YO10 5DD, U.K.
⁶ School of Chemistry, University of Glasgow, Glasgow G12 8QQ, U.K.

Abstract

Self-assembled nanofibers are ubiquitous in nature and serve as inspiration for the design of supramolecular hydrogels. A multicomponent approach offers the possibility of enhancing the tunability and functionality of this class of materials. We report on the synergistic multicomponent self-assembly involving a peptide amphiphile (PA) and a 1,3:2,4-dibenzylidene-d-sorbitol (DBS) gelator to generate hydrogels with tunable nanoscale morphology, improved stiffness, enhanced self-healing, and stability to enzymatic degradation. Using induced circular dichroism of Thioflavin T (ThT), electron microscopy, small-angle neutron scattering, and molecular dynamics approaches, we confirm that the PA undergoes self-sorting, while the DBS gelator acts as an additive modifier for the PA nanofibers. The supramolecular interactions between the PA and DBS gelators result in improved bulk properties and cytocompatibility of the two-component hydrogels as compared to those of the single-component systems. The tunable mechanical properties, self-healing ability, resistance to proteolysis, and biocompatibility of the hydrogels suggest future opportunities for the hydrogels as scaffolds for tissue engineering and drug delivery vehicles.