How bulk liquid viscosity shapes capillary suspensions

Capillary suspensions offer a new approach to generate novel materials. They are ternary liquid-liquid-solid systems characterized by particles connected by liquid bridges of one fluid suspended in a second immiscible bulk fluid. The viscosity of the bulk liquid can be modulated to customize the structure and rheological properties of capillary suspensions. Experiments and simulations: Using experiments and numerical simulations, we investigated capillary suspensions in the pendular state, using silica particles and water as a bridging liquid. To modulate the viscosity of the bulk fluid, we use different ratios of either dodecane and diisononyl phthalate, or silicone oils with varying chain lengths as bulk liquids. The rheological behavior was characterized using the maximum storage and loss moduli and the yielding behavior. This was related to structural changes of the systems, which was visualized using confocal laser scanning microscopy. In addition, we used Molecular Dynamics (MD) simulations to gain more insights into the behavior of two particles connected by a liquid bridge for various bulk liquids.

Experiments show that higher bulk liquid viscosity reduces strength, yield stress, and yield strain in capillary suspensions, which is partly attributed to a reduced inter-connectivity of the percolating network. This is caused by the breakup of liquid bridges occurring at shorter distances in the presence of highly viscous bulk liquids, as indicated by numerical simulations.