Deconvolution of electrochemical impedance spectra for the identification of electrode reaction mechanisms in solid oxide fuel cells

Abstract

The polarization processes occurring at the electrode–electrolyte interfaces of solid oxide fuel cells (SOFC) were investigated by electrochemical impedance spectra measured at single cells under realistic operating conditions. The approach presented is based on distributions of relaxation times which are the basic quantity of interest in electrochemical impedance data analysis. A deconvolution method was developed and implemented that yields these characteristic distribution patterns directly from the impedance spectra. In contrast to nonlinear least squares curve fit of equivalent circuit models, no a priori circuit choice has to be made. Even more importantly, the excellent resolving capacity allows the untangling of the impedance contributions of up to three physically distinct processes within one frequency decade. With the method, processes with the highest polarization losses can be identified and targeted to improve cell performance. Based on the distributions, a general strategy for the identification of the reaction mechanisms is given. The evaluation of the distributions in terms of peak parameters is illustrated by a physical model for oxygen reduction at the SOFC cathode–electrolyte interface. The method is expected to find many applications in electrochemistry beyond the field of solid oxide fuel cell development.