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The non-Newtonian behaviors of dense suspensions are central to their use intechnological and industrial applications and arise from a network ofparticle-particle contacts that dynamically adapts to imposed shear. Reportedherein are studies aimed at explor-ing how dynamic covalent chemistry betweenparticles and the polymeric solvent can be used to tailor such stress-adaptivecontact networks leading to their unusual rheological behaviors. Specifically,a room temperature dynamic thia-Michael bond is employed to rationally tune theequilibrium constant (Keq) of the polymeric solvent to the particle interface.It is demonstrated that low Keq leads to shear thinning while high Keq producesantithixotropy, a rare phenomenon where the viscosity increases with shearingtime. It is proposed that an increase in Keq increases the polymer graftdensity at the particle surface and that antithixotropy primar-ily arises frompartial debonding of the polymeric graft/solvent from the particle surface andthe formation of polymer bridges between particles. Thus, the implementation ofdynamic covalent chemistry provides a new molecular handle with which to tailorthe macroscopic rheology of suspensions by introducing programable timedependence. These studies open the door to energy absorbing materials that notonly sense mechanical inputs and adjust their dissipation as a function of timeor shear rate but can switch between these two modalities on demand.

Designing Stress-Adaptive Dense Suspensions using Dynamic Covalent Chemistry