A structural model for yielding and degelation of hydrogels

Zelai Xu & James J. Feng

J. Rheol. (submitted 2025)

Abstract - Yielding is observed for a wide range of soft materials. For colloidal gels, recent experiments and Brownian dynamics simulations have revealed intriguing new features, including delayed yielding and degelation, characterized by distinct temporal evolutions of the strain and strain rate in creep tests. The objective of this work is to encapsulate such features in a compact continuum-level rheological model suitable for flow simulations. The model has three core components: (i) a degelation criterion that reflects a sharp sol-gel transition; (ii) a structural parameter that represents the degree of bonding in the gel, whose evolution is dictated by bond breakage under deformation and formation of new bonds; (iii) a dynamically evolving elastic strain that represents the state of elastic stress and energy in the gel. Applied to simple shear flows under a constant stress (creep), startup of simple shear and pressure-driven Poiseuille flow in a circular tube, the model predicts three regimes with increasing stress: non-yielding, yielding and degelation. The transition between neighboring regimes exhibits hysteresis. The hysteresis between the yielding and degelation regimes resembles that in micellar solutions, and shear-banding occurs at a uniquely selected stress when diffusion is allowed across the boundary between the bands. These predictions are in qualitative agreement with experiments.