C_xN_y particles@N-doped porous graphene: a novel cathode catalyst with a remarkable cyclability for Li-O₂ batteries

Despite the intrinsic advantages of ultra-high theoretical capacity and energy density of lithium-O2 batteries, there remain several critical issues to be resolved, especially the two concerning poor cyclability and rate capability. In this work, CxNy particles@N-doped porous graphene (CxNy@NPG) with a novel three-dimensional architecture is successfully synthesized via a simple template method and employed as the cathode catalyst of Li-O2 batteries. It is surprisingly found that the as-synthesized CxNy@NPG cathode not only demonstrates a remarkable cycling performance of 200 cycles at 1000 mA g-1 but also an intriguing high-rate capability with 8892 mA h g-1 at 1000 mA g-1, both of which can be attributed to a synergistic effect between the unique 3D porous structure and an effective N-doping. Specifically, it is believed that the unique porous 3D structure will, on one hand, build numerous microchannels, thus facilitating rapid O2 diffusion, and on the other hand, provide sufficient storage space to accommodate adequate discharge products. Indispensably, it is also believed that the N-doped porous graphene enables improved bifunctional catalytic activities towards both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), thus decreasing the discharge/charge overpotential, and reducing undesired side reactions. It is anticipated that the new 3D porous CxNy@NPG provides an inspiring route to design long cycling and high-rate performance cathodes for Li-O2 batteries.