Well-defined synthetic copolymers with pendant aldehydes form biocompatible strain-stiffening hydrogels and enable competitive ligand displacement

Subsequently, we observed fast gelation kinetics with imine-type crosslinking. We were able to vary hydrogel stiffness from ≈ 2–20 kPa, tune the onset of strain-stiffening towards a biologically relevant regime (σc ≈ 10 Pa), and demonstrate cytocompatibility using human dermal fibroblasts. Moreover, to begin to mimic the dynamic biochemical nature of the native ECM, we highlight the potential for temporal modulation of ligands in our system to demonstrate ligand displacement along the copolymer backbone via competitive binding.

The combination of highly tunable composition, stiffness, and strain-stiffening, in conjunction with spatiotemporal control of functionality, positions these cytocompatible copolymers as a powerful synthetic platform for the rational design of next-generation synthetic biomaterials.