Novel viscoelastic smart suspensions based on cationic wormlike micelles (WLMs) of erucylbis(hydroxyethyl)methylammonium chloride and oppositely charged submicron magnetite particles in the presence of added low molecular weight salt were prepared and investigated. The suspensions demonstrate remarkable stability against sedimentation, which can be due to the incorporation of particles into the network of entangled WLMs by linking to energetically unfavorable micellar end-caps. Added particles enhance significantly the viscosity, the plateau modulus, and the relaxation time of the system, acting as additional multifunctional physical cross-links in the micellar network. The increase of plateau modulus stops when the concentration of particles reaches ca. 1.5 wt %, indicating that all micellar end-caps available in the system are linked to the particles. Further addition of particles may lead just to the redistribution of micellar ends between the particles without creation of new elastically active chains. The increase of rheological characteristics by added particles is more pronounced in suspensions with a smaller content of low molecular weight salt KCl when the WLMs are shorter in length and therefore contain a larger amount of end-caps responsible for the interaction with the particles. Magnetite particles not only enhance the rheological characteristics but also impart magnetoresponsive properties to the suspension. Upon application of magnetic field, the liquidlike system transforms into a solidlike one, demonstrating a constant value of storage modulus in all frequency range and the appearance of yield stress, which is due to the formation of field-aligned chainlike aggregates of particles opposing the flow. A combination of responsive properties inherent to both the matrix and the particles makes these smart fluids very competitive with other magnetic soft matter materials for various applications.
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