Aerophilic Triphase Interface Tuned by Carbon Dots Driving Durable and Flexible Rechargeable Zn-Air Batteries

Efficient bifunctional catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are vital for rechargeable Zn-air batteries (ZABs). Herein, an oxygen-respirable sponge-like Co@C-O-Cs catalyst with oxygen-rich active sites was designed and constructed for both ORR and OER by a facile carbon dot-assisted strategy. The aerophilic triphase interface of Co@C-O-Cs cathode efficiently boosts oxygen diffusion and transfer. The theoretical calculations and experimental studies revealed that the Co-C-COC active sites can redistribute the local charge density and lower the reaction energy barrier. The Co@C-O-Cs catalyst displays superior bifunctional catalytic activities with a half-wave potential of 0.82 V for ORR and an ultralow overpotential of 294 mV at 10 mA cm^-2 for OER. Moreover, it can drive the liquid ZABs with high peak power density (106.4 mW cm^-2), specific capacity (720.7 mAh g^-1), outstanding long-term cycle stability (over 750 cycles at 10 mA cm^-2), and exhibits excellent feasibility in flexible all-solid-state ZABs. These findings provide new insights into the rational design of efficient bifunctional oxygen catalysts in rechargeable metal-air batteries.