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Hydrogels are soft materials engineered to suit a multitude of applicationsthat exploit their tunable mechanochemical properties. Dynamic hydrogelsemploying noncovalent, physically crosslinked networks dominated by eitherenthalpic or entropic interactions enable unique rheological andstimuli-responsive characteristics. In contrast to enthalpy-driven interactionsthat soften with increasing temperature, entropic interactions result inlargely temperature-independent mechanical properties. By engineeringinterfacial polymer-particle interactions, we can induce a dynamic-to-covalenttransition in entropic hydrogels that leads to biomimetic non-ergodic aging inthe microstructure without altering the network mesh size. This transition istuned by varying temperature and formulation conditions such as $p$H, whichallows for multivalent tunability in properties. These hydrogels can thus bedesigned to exhibit either temperature-independent metastable dynamiccrosslinking or time-dependent stiffening based on formulation and storageconditions, all while maintaining strucutural features critical for controllingmass transport, akin to many biological tissues. Such robust materials withversatile and adaptable properties can be utilized in applications such aswildfire suppression, surgical adhesives, and depot-forming injectable drugdelivery systems.

Biomimetic non-ergodic aging by dynamic-to-covalent transitions in physical hydrogels