Native protein hydrogels by dynamic boronic acid chemistry

Bioactive protein-based materials are unique functional systems that incorporate the specificity and intelligent characteristics of biomolecules within synthetic polymers. Herein, we take advantage of the boronic acid/salicyl hydroxamate molecular recognition strategy to crosslink an apoptosis inducing enzyme, cytochrome c, by dynamic covalent interactions to form a bioactive and responsive hydrogel for controlled administration. The material exhibits attractive rheological properties with high storage modulus and modulus crossover despite the perceived conformational sensitivity of the proteins. Upon acidification, the hydrogel matrix dissociated and release active enzymes into A549 cells, which initiates apoptosis. In combination, the chemical strategy facilitates the integration of native enzymes structurally into the hydrogel scaffold while simultaneously providing biological activity under a stimulus controlled release mechanism.

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