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Aqueous lithium–oxygen batteries are promising candidates for electric energy storage. In this paper we present and discuss a multiphase continuum model of an aqueous lithium–oxygen single cell including reactions and transport in a porous gas diffusion electrode (GDE). The model is parameterized using in-house half-cell experiments and available literature data on aqueous electrolytes. We validate our transport model with cyclic voltammetry and electrochemical impedance spectroscopy measurements over a wide range of temperatures (25, 40, 55 °C) and electrolyte concentrations (0.1–2 M). We observe very good agreement between simulations and measurements during oxygen reduction conditions. A sensitivity analysis of the validated model demonstrates the influence of the porous structure on GDE performance and gives directions for the future development of electrodes.
A wide range catalyst screening with noble metal and oxide catalysts for a metal–air battery with an aqueous alkaline electrolyte was carried out. Suitable catalysts reduce overpotentials during the charge and discharge process, and therefore improve the round-trip efficiency of the battery. In this case, the electrodes will be used as optimized cathodes for a future lithium–air battery with an aqueous alkaline electrolyte. Oxide catalysts were synthesized via atmospheric plasma spraying. The screening showed that IrO2, RuO2, La0.6Ca0.4Co3, Mn3O4, and Co3O4 are promising bi-functional catalysts. Considering the high price for the noble metal catalysts further investigations of the oxide catalysts were carried out to analyze their electrochemical behavior at varied temperatures, molarities, and in case of La1−x Ca x CoO3 a varying calcium content. Additionally all catalysts were tested in a longterm test to proof cyclability at varied molarities. Further investigations showed that Co3O4 seems to be the most promising bi-functional catalyst of the tested oxide catalysts. Furthermore, it was shown that a calcium content of x = 0.4 in LCCO has the best performance.