Nitrogen-Doped Holey Graphene for High-Performance Rechargeable Li-O₂ Batteries

Li-air batteries represent cutting edge electrochemical energy storage devices, but their practical applications have been precluded by the high cathode cost, the low discharge/charge efficiency, and/or the short battery lifetime. Here, we developed a low-cost, but very efficient, air electrode from porous nitrogen-doped holey graphene for rechargeable nonaqueous Li-O₂ cells. The resultant Li-O₂ cell can deliver a high round-trip efficiency (85%) and a long cycling life (>100 cycles) under controlled discharge/charge depths or a high capacity of 17000 mAh/g under the full discharge/charge condition, superior to most other carbonaceous air cathodes. The observed superb performance for the air electrode based on the nitrogen-doped holey graphene can be attributed to its efficient metal-free catalytic activity and three-dimensional mass transport pathway. Therefore, this work represents a new approach to low-cost, efficient, metal-free, binder-free, and hierarchically porous air electrodes useful for energy conversion and storage from N-doped holey graphene.