In order to gain insight on the physical processes governing cell performance, we have used nonlinear electrochemical impedance spectroscopy (NLEIS) to probe the nonlinear harmonic current-voltage characteristics of a LaxSr1-xCoO3-δ electrode. Harmonic spectra acquired over a range of conditions were compared to a theoretical model that considers the relative roles of material thermodynamics, surface exchange reaction and ion diffusion within a cylindrical electrode particle. For a Strontium dopant content of 0.4, a comparison of the theoretical and experimental nonlinearities suggests that the cell behavior is not consistent with a purely bulk-diffusion limited mechanism. This result is contrary to linear impedance observations and suggests that the nonlinear behavior could be influenced by an alternative surface diffusion mechanism or material thermodynamics.