Direct Evidence of Electric Double Layer (EDL) Repulsive Force Being Responsible for the Time-Dependent Behavior of Clay Gels in the Structural Rejuvenation Mode.

A strong EDL repulsive force is needed to accentuate the time-dependent behavior of charge and shape anisotropic clay gels at the stepdown shear rate. This force was strengthened by PO adsorption, increasing the negative charge density of the clay particles. At the stepdown shear rate of 10 s, it is strong enough to disrupt the flow-aligned structure attained at 1000 s and orient the particles to form more bonds. The resultant outcome is stepdown shear stress increasing with time until these structure disruption and bond formation processes reach an equilibrium state. The number of lower energy approach configurations (-ve face - +ve edge) for bonding is reduced by the strengthened EDL repulsive force, slowing the bonding process. The time to reach the equilibrium stepdown shear stress value increased initially and then decreased and became zero at a high negative charge density where the charge anisotropy of the particles no longer exists. The need of a sufficiently strong EDL repulsive force for the display of time-dependent behavior is true for all clay gels: Laponite, hectorite, NaMnt, sepiolite, and kaolin gels. The untreated NaMnt gel already displayed time-dependent behavior as its EDL repulsive force is sufficiently strong. The same EDL-control time-dependent behavior was obtained if pH was used to vary the negative charge density of the clay particles.