Modeling the impedance response and steady state behaviour of porous CGO-based MIEC anodes

Phys Chem Chem Phys. 2021 Oct 20;23(40):23042-23074. doi: 10.1039/d1cp01962g.

Abstract

Mixed ionic and electronic conducting (MIEC) materials recently gained much interest for use as anodes in solid oxide fuel cell (SOFC) applications. However, many processes in MIEC-based porous anodes are still poorly understood and the appropriate interpretation of corresponding electrochemical impedance spectroscopy (EIS) data is challenging. Therefore, a model which is capable to capture all relevant physico-chemical processes is a crucial prerequisite for systematic materials optimization. In this contribution we present a comprehensive model for MIEC-based anodes providing both the DC-behaviour and the EIS-spectra. The model enables one to distinguish between the impact of the chemical capacitance, the reaction resistance, the gas impedance and the charge transport resistance on the EIS-spectrum and therewith allows its appropriate interpretation for button cell conditions. Typical MIEC-features are studied with the model applied to gadolinium doped ceria (CGO) anodes with different microstructures. The results obtained for CGO anodes reveal the spatial distribution of the reaction zone and associated transport distances for the charge carriers and gas species. Moreover, parameter spaces for transport limited and surface reaction limited situations are depicted. By linking bulk material properties, microstructure effects and the cell design with the cell performance, we present a way towards a systematic materials optimization for MIEC-based anodes.