Functional nano or microparticles in solution can form stimuli-responsive smart fluids that exhibit drastic property changes in the presence of magnetic or electric fields that originate from the interparticle interactions. For example, the most commonly utilized type of particle-based smart fluid are magnetorheological fluids (MRF) that contain ferromagnetic microparticles that allow them to reversibly solidify when they experience a magnetic field. The tunable nature of these materials not only make them useful in a variety of industries, but also make them a versatile system in which to study the influence of interparticle interactions on emergent behaviors. In this dissertation, we explore methods for tuning interparticle interactions with applied fields, additives, and functionalized particles and develop, through both experimentation and modeling, design rules for realizing new classes of smart fluids.
First, we address a common limitation on the performance of MRF, namely slip failure, through the use of a shear-thickening additive to reinforce MRF particle chains as slip begins. Through flow- and oscillation-mode rheology, we find that a shear-thickening MRF has 60% higher yield stress than a conventional shear-thinning MRF. The shear-thickening additive allows us to affect the microstructure of the fluid in order to increase bulk performance by changing its failure mode.
Next, we explore the hypothesis that highly anisotropic 2D sheets can reinforce conventional MRF as an additive by supporting the particle chains. Interestingly, the 2D sheets affect the performance of the fluid minimally in a boundary-driven flow because of the alignment of the sheets in the fluid velocity profile. However, we find that the 2D sheets increase MRF performance in pressure-driven flows by up to 45%. We determine through modeling that this performance improvement stems from the anisotropic sheets physically reinforcing the particle chains. This work has consequences for the design of MRF for applications using pressure-driven flows, such as soft robotics.
In addition to studying the additives as a path to strengthening MRF, we investigate whether the magnetic particles themselves can be modified to chemically adhere to one another, thus providing additional attractive forces to supplement the magnetic force between particles. Using flow- and oscillation-mode rheology, we quantify the performance using both the yield stress and chain stiffness as performance metrics. By developing two different adhesive MRF, we find that linked chains exhibit a 40% increase in yield stress and a 100% increase in stiffness. Using thymine-functionalized particles, we present a dynamic method for linking particles in an MRF for increased performance.
Finally, a system of polarizable nanoparticles is investigated after it is observed to exhibit a macroscopic cellular phase with particle-poor voids and particle-rich walls in a fluid cell when applying an AC and DC field. By tuning the applied AC and DC fields, we identify the conditions necessary for the phase transition using fluorescence microscopy. We also find through Cahn-Hilliard analysis and additional experiments that the cellular phase is the result of various types of electrically-induced interactions. Specifically, electrophoresis causes the particles to accumulate on one electrode, then electroosmotic and electrohydrodynamic flows occur and exert attractive and repulsive forces on the particles. When the electrohydrodynamic flow dominates, voids nucleate at high field regions at which point spinodal decomposition into the cellular phase occurs. This understanding allows us to explore ways to tune this behavior such as using photolithography to control the location of the voids, and thus the structure of the material
