Hierarchical Nitrogen‐Doped Graphene/Carbon Nanotube Composite Cathode for Lithium–Oxygen Batteries

Abstract The lithium–oxygen (Li–O 2 ) battery is a very appealing candidate for advanced high energy applications owing to its exceptionally high specific energy. However, its poor energy efficiency, rate capability, and cyclability remain key barriers to its practical application. In this work, using a rationally designed cathode based on a bimodal mesoporous nitrogen‐doped graphene/carbon nanotube (NGC) composite, we have developed a Li–O 2 battery demonstrating enhanced round‐trip efficiency (ca. 85 %) and excellent cyclability over 400 cycles under a high current rate of 500 mA g −1 . The excellent cyclability and rate capability are attributed to improved stability of the aggressive LiO 2 intermediate on the nitrogen‐doped carbon surface in addition to the favorable hierarchical architecture of NGC. These results demonstrate a valuable research direction to achieve highly stable and reversible Li–O 2 batteries through tuning the surface chemistry of the cathode in addition to finding a stable electrolyte solvent.