Granular Hydrogels as Brittle Yield Stress Fluids

While granular hydrogels are increasingly used in biomedical applications, methods to capture their rheological behavior generally consider shear‐thinning and self‐healing properties or produce ensemble metrics (e.g., dynamic moduli) while neglecting transient yielding and unyielding processes. Combining oscillatory shear testing with Brittility (Bt) via the Kamani‐Donley‐Rogers (KDR) model, this work shows that granular hydrogels behave as brittle yield stress fluids. This work quantifies steady and transient rheology as a function of microgel properties and granular composition for polyethylene glycol and gelatin microgels. The KDR model with Bt captures granular hydrogel behavior for a wide range of design parameters, reducing the complex rheology to a determination of model parameters. In granular mixtures, this work observes monotonic dependencies of the elastic modulus, structural viscosity, and brittility upon granular composition, while the yield stress is lower for mixtures. Microgel size distribution and polymer fraction are the most influential parameters in monolithic granular hydrogels, while microgel size and packing density are less impactful. The model robustly captures self‐healing behavior and reveals that granular hydrogel relaxation accelerates with an increased small‐amplitude strain rate. This quantitative framework is an important step toward rational design of granular hydrogels for applications ranging from injection and in situ stabilization to 3D bioprinting.