Li-CO batteries are explored as promising power systems to alleviate environmental issues and to implement space applications. However, sluggish cathode kinetics of CO reduction/evolution result in low round-trip efficiency and poor cycling stability of the fabricated energy-storage devices. Herein, we design a heterostructued photocathode comprising carbon nanotube and carbon nitride to accelerate cathode reactions of a Li-CO battery under illumination. Benefiting from the unique defective structure of carbon nitride and favorable interfacial charge transfer, the photocathode effectively harvests ultraviolet-visible light to generate abundant photoexcited carriers and coordinates energetic photoelectrons/holes to participate in the discharge/charge reactions, leading to efficient photo-energy utilization in decreasing reaction barriers and enhancing thermodynamic reversibility of Li-CO battery. The resulting battery delivers a high round-trip efficiency of 98.8 % (ultralow voltage hysteresis of 0.04 V) and superior cycling stability (86.1 % efficiency retention after 100 cycles).
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