Hierarchical Carbon–Nitrogen Architectures with Both Mesopores and Macrochannels as Excellent Cathodes for Rechargeable Li–O2 Batteries

Lithium–oxygen batteries are attracting more and more interest; however, their poor rechargeability and low efficiency remain critical barriers to practical applications. Herein, hierarchical carbon–nitrogen architectures with both macrochannels and mesopores are prepared through an economical and environmentally benign sol–gel route, which show high electrocatalytic activity and stable cyclability over 160 cycles as cathodes for Li–O 2 batteries. Such good performance owes to the coexistence of macrochannels and mesopores in C–N hierarchical architectures, which greatly facilitate the Li + diffusion and electrolyte immersion, as well as provide an effective space for O 2 diffusion and O 2 /Li 2 O 2 conversion. Additionally, the mechanism of oxygen reduction reactions is discussed with the N‐rich carbon materials through first‐principles computations. The lithiated pyridinic N provides excellent O 2 adsorption and activation sites, and thus catalyzes the electrode processes. Therefore, hierarchical carbon–nitrogen architectures with both macrochannels and mesopores are promising cathodes for Li–O 2 batteries.