ABSTRACT

We consider a mixture made of dispersed metallic particles immersed into a background material saturated by an electrolyte. Below the freezing temperature (typically 0°C to 4°C), a fraction of the liquid water in the pore space is transformed into ice, whereas the salt remains segregated into the liquid-pore water solution. Our goal is to understand how freezing affects the complex conductivity (induced polarization) of such mixtures. Complex conductivity measurements (96 spectra) are performed in a temperature-controlled bath equipped with a high-precision impedance meter. We cover the temperature range from +20°C to 15°C to 18°C and the frequency range from 102  Hz to 45 kHz. The spectra are fitted with a double Cole-Cole complex conductivity model. A finite-element model is used to further analyze the mechanisms of polarization by considering an intragrain polarization mechanism for the metallic particles and a change of the conductivity of the background material modeled with an exponential freezing curve. This curve is used to relate the liquid water content to the temperature. In the context of freezing, we test all the aspects of the intragrain polarization model developed in the previous papers of this series, at least for a weakly polarizable background material. The Cole-Cole exponent and the chargeability are observed to be essentially independent of temperature including in freezing conditions. This means that all the relaxation times of the system follow the same temperature dependence and that the chargeability is controlled by the volume fraction of metal. The instantaneous conductivity (high-frequency conductivity) and the relaxation times depend on the temperature in a predictable way, and their product can be considered to be essentially temperature independent. The analytical and numerical models can reproduce the inverse relationship between the relaxation time and the instantaneous conductivity.

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