Simultaneous Rheoelectric Measurements of Strongly Conductive Complex Fluids

We introduce an modular fixture designed for stress-controlled rheometers to perform simultaneous rheological and electrical measurements on strongly conductive complex fluids under shear. By means of a nontoxic liquid metal at room temperature, the electrical connection to the rotating shaft is completed with minimal additional mechanical friction, allowing for simultaneous stress measurements at values as low as 1 Pa. Motivated by applications such as flow batteries, we use the capabilities of this design to perform an extensive set of rheoelectric experiments on gels formulated from attractive carbon-black particles, at concentrations ranging from 4 to 15 wt %. First, experiments on gels at rest prepared with different shear histories show a robust power-law scaling between the elastic modulus G(0)' and the conductivity sigma(0) of the gels-i.e., G(0)' similar to sigma(alpha)(0), with alpha = 1.65 +/- 0.04, regardless of the gel concentration. Second, we report conductivity measurements performed simultaneously with creep experiments. Changes in conductivity in the early stage of the experiments, also known as the Andrade-creep regime, reveal for the first time that plastic events take place in the bulk, while the shear rate gamma decreases as a weak power law of time. The subsequent evolution of the conductivity and the shear rate allows us to propose a local yielding scenario that is in agreement with previous velocimetry measurements. Finally, to establish a set of benchmark data, we determine the constitutive rheological and electrical behavior of carbon-black gels. Corrections first introduced for mechanical measurements regarding shear inhomogeneity and wall slip are carefully extended to electrical measurements to accurately distinguish between bulk and surface contributions to the conductivity. As an illustrative example, we examine the constitutive rheoelectric properties of five different grades of carbon-black gels and we demonstrate the relevance of this rheoelectric apparatus as a versatile characterization tool for strongly conductive complex fluids and their applications.