Injectable organo- and hydrogels are desired in many biomedical applications due to minimally invasive application and their ability to co-inject functional additives such as drugs and contrast agents. However, current injectables suffer from mechanical mismatch with tissue and uncontrolled swelling. Herein, we design brush-like macromolecules that concurrently provide softness, firmness, strength, fluidity, and swellability. The synthesized linear-bottlebrush-linear copolymers where the brush block facilitates injectability and softness while the thermo-responsive linear blocks permit prompt gelation at 37°C. The resulting hydrogels mimic the deformation response of soft tissues, while withstanding deformations of 700% and precluding water expulsion upon gelation. Furthermore, brush architecture allows independent variation of elastic modulus and equilibrium swelling ratio of polymer networks. By coordinating grafting density and side chain length, we prepare gels with the same equilibrium solvent fraction yet vastly different stiffness’. The design-by-architecture approach is universally applicable to both organogels and hydrogels with multiple implications in both medical and non-medical technologies.

Injectable bottlebrush gels with tissue-mimetic mechanics and swellability

ACS Spring 2022

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