Abstract
We present a theoretical analysis of the 1st, 2nd, and 3rd order harmonic voltage response of a dense thin-film SOFC cathode to a sinusoidal current perturbation. Our analysis shows that significant variations in the rate determining physics can yield very similar response in the 1st harmonic (impedance), making it potentially difficult to discern mechanism directly from impedance measurements alone. However, these same variations produce significant differences in the 2nd and 3rd order harmonic responses, illustrating the possible usefulness of measuring harmonics as a way of distinguishing physical processes. We lay out a general framework for calculating these responses numerically based on a given mechanistic model for the electrode reaction.
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