Tuning the Hierarchical Structure and Resilience of Resilin-like Polypeptide Hydrogels Using Graphene Oxide

Resilin-like polypeptides (RLPs) are an important class of intrinsically disordered multistimuli-responsive bioelastomers. The nanostructure of RLPs in solution has been extensively studied in the past few years, from dilute to molecular crowding conditions, and with the addition of rigid biopolymers. Modification of the hierarchical network structure of RLP hydrogels using graphene oxide (GO) as an additive is a burgeoning prospect for their application in the bioelectronic and biomedical fields. In this work, we systemically study the influence of incorporating GO into RLP (Rec1) hydrogels for tuning their physicochemical properties and understanding the gel-cell interactions. The nature of GO interaction with the Rec1 hydrogel is deduced from the change in structure and properties. Contrast-matching small-angle and ultra-small-angle neutron-scattering techniques were used to investigate the network structure of the Rec1 hydrogel and how this structure is modified in the presence of GO. Incorporation of GO in the Rec1 hydrogel matrix results in an increase in the micromechanical resilience, equilibrium water swelling ratio, micropore size, cross-linked domain size; with a decrease in the cross-link density, mass fractal cluster size, local compressive elastic modulus, and cell inert characteristics. These property combinations achieved with the addition of GO further open up the available structure-property design window for RLP applications.