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In this paper we use continuum modeling to analyze the mechanism of the oxygen reduction reaction at a porous mixed-conducting oxygen electrode. We show that for La0 5(Ca, Sr)04Fe08Co0203,, at 700°C, solid-state oxygen diffusion and 02 surface exchange dominate the electrochemical behavior, producing effective "chemical" resistances and capacitances. This behavior can be explained both qualitatively and quantitatively in terms of the known bulk and surface properties of the materials. This mechanism appears to be generally valid for mixed conductors with high rates of internal mass transfer, but breaks down for mixed conductors that have poor ionic transport. Our analysis also suggests that, for the best electrode materials, extension of the reaction zone beyond the three-phase boundary is limited to a few micrometers. We also show that gas phase diffusion resistance can contribute significantly to cell impedance at P0 0.1 atm. InfroductionElectrode reactions in solid-state electrochemical systems involve a complex interaction of mobile electronic, ionic, and molecular species. One example that has drawn

The drive towards increased energy efficiency and reduced air pollution has led to accelerated worldwide development of fuel cells. As the performance and cost of fuel cells have improved, the materials comprising them have become increasingly sophisticated, both in composition and microstructure. In particular, state-of-the-art fuel-cell electrodes typically have a complex micro/nano-structure involving interconnected electronically and ionically conducting phases, gas-phase porosity, and catalytically active surfaces. Determining this microstructure is a critical, yet usually missing, link between materials properties/processing and electrode performance. Current methods of microstructural analysis, such as scanning electron microscopy, only provide two-dimensional anecdotes of the microstructure, and thus limited information about how regions are interconnected in three-dimensional space. Here we demonstrate the use of dual-beam focused ion beam-scanning electron microscopy to make a complete three-dimensional reconstruction of a solid-oxide fuel-cell electrode. We use this data to calculate critical microstructural features such as volume fractions and surface areas of specific phases, three-phase boundary length, and the connectivity and tortuosity of specific subphases.

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