Li-O batteries are considered the ultimate energy storage technology for their potential to store large amounts of electrical energy in a cost-effective and simple platform. Large overpotentials for the formation and oxidation of LiO during discharging and charging have thus far confined this technology to a scientific curiosity. Herein, we consider the role of catalytic intervention in the reversibility of the cathode reactions and find that semiconducting metal-organic polymer nanosheets composed of cobalt-tetramino-benzoquinone (Co-TABQ) function as a bifunctional catalyst that facilitates the kinetics of the cathode reactions under visible light. Upon discharging, we report that O is first adsorbed on the Co atoms of Co-TABQ and accepts electrons under illumination from the d and d orbitals of Co atoms in the π orbitals, which facilitates reduction to LiO. The LiO is further shown to undergo a second reduction to the discharge product of LiO. In the reverse charge, the holes generated in the d orbitals of Co are mobilized under the action of the applied voltage to enable the fast decomposition of LiO to O and Li. Under illumination, the Li-O battery exhibits respective discharge and charge voltages of 3.12 and 3.32 V for a round-trip efficiency of 94.0%. Our findings imply that the orbital interaction of metal ions with ligands in Co-TABQ nanosheets dictates the light harvesting and oxygen electrocatalysis for the Li-O battery.
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