Filled Colloidal Gel Rheology: Strengthening, Stiffening, and Tunability

Filler-induced strengthening is ubiquitous in materials science and is particularly well-established in polymeric nanocomposites. Despite having similar constituents, colloidal gels with solid filling exhibit distinct rheology, which is of practical interest to industry (e.g., lithium-ion batteries) yet remains poorly understood. We show, using experiments and simulations, that filling monotonically enhances the yield stress (i.e., strength) of colloidal gels while the elastic modulus (i.e., stiffness) first increases and then decreases. The latter softening effect results from a frustrated gel matrix at dense filling, evidenced by a growing inter-phase pressure. This structural frustration is, however, not detrimental to yielding resistance. Instead, fillers offer additional mechanical support to the gel backbone via percolating force chains, decreasing the yield strain at the same time. We develop a mechanistic picture of this phenomenology that leads us to a novel `filler-removal protocol,' making individual control over the strength and brittleness of a composite gel possible.