Influence of the Oxygen Electrode Open Ratio and Electrolyte Evaporation on the Performance of Li–O₂ Batteries

Abstract

This study experimentally investigates and numerically simulates the influence of the cathode electrode open ratio (ratio of oxygen-opening area to the total electrode surface area) on the performance of Li-O batteries at various discharge current densities. At the current density of 0.1 mA/cm, the maximum discharge capacity is achieved at 25% open ratio among the tested open ratios (0-100%). As the open ratio increases from 25% to 100%, the specific discharge capacity decreases from 995 to 397 mA h/g. A similar trend is observed at 0.3 mA/cm, while the maximum discharge capacity is obtained at 3% open ratio among the tested open ratios. The model that assumes the electrode is always fully saturated by the electrolyte does not obtain similar trends with experimental results, while the model that considers electrolyte loss by evaporation and the volume change of the solid obtains the same trend with experimental observations. The open ratio governs not only availability of oxygen but also the evaporation of the electrolyte and the contact resistance. The faster evaporation of the electrolyte at a higher open ratio can be the main reason for the decrease of the discharge capacity, especially when the open ratio is relatively high (above 25%). Meanwhile, the contact resistance of the battery, measured by the electrochemical impedance spectroscopy (EIS), increases from 3.97 to 7.02 Ω when the open ratio increased from 3% to 95%. The increase of the Ohmic overpotential, however, is negligible (on the order of millivolts) because of the low discharge and charge current rates (on the order of 0.1 mA).

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