Abstract

AbstractLi–O2batteries have aroused considerable interest in recent years, however they are hindered by high kinetic barriers and large overvoltages at cathodes. Herein, a step‐scheme (S‐scheme) junction with hematite on carbon nitride (Fe2O3/C3N4) is designed as a bifunctional catalyst to facilitate oxygen redox for a visible‐light‐involved Li–O2battery. The internal electric field and interfacial Fe−N bonding in the heterojunction boost the separation and directional migration of photo‐carriers to establish spatially isolated redox centers, at which the photoelectrons on C3N4and holes on Fe2O3remarkably accelerate the discharge and charge kinetics. These enable the Li–O2battery with Fe2O3/C3N4to present an elevated discharge voltage of 3.13 V under illumination, higher than the equilibrium potential 2.96 V in the dark, and a charge voltage of 3.19 V, as well as superior rate capability and cycling stability. This work will shed light on rational cathode design for metal–O2batteries.

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