The role of catalysts in aprotic Li−O 2 batteries remains unclear. To identify the exact catalytic nature of oxide catalysts, a precisely surface-engineered model catalyst, perovskite (LaMnO 3 ), was investigated for oxygen reduction reaction/ oxygen evolution reaction (ORR/OER) in both aqueous and aprotic solutions. By using integrated theoretical and experimental approaches, we explicitly show that H + -ORR/OER catalytic activity on transition-metal sites fails to completely describe the electrochemical performance of LaMnO 3 catalysts in aprotic Li−O 2 batteries, whereas the collective redox of the lattice oxygen and transition metal on the catalyst surface during initial Li 2 O 2 formation determines their discharge capacity and charge overpotential. This work applies oxide catalyst design to tailor both the surface lattice oxygen and the transition-metal arrangement for an aprotic Li−O 2 battery. The optimized model catalyst shows good performance for Li−O 2 batteries under both oxygen and ambient air (real air) conditions.
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