Constructing Pentagonal Topological Defects in Carbon Aerogels for Flexible Zinc‐Air Batteries

Abstract In the context of energy conversion, the design and synthesis of high‐performance metal‐free carbon electrocatalysts for the oxygen reduction reaction (ORR) is crucial. Herein, a one‐step nitrogen doping/extraction strategy is proposed to fabricate 3D nitrogen‐doped carbon aerogels (NCA‐Cl) with rich pentagonal carbon topological defects. The NCA‐Cl electrocatalyst exhibits superb ORR activity, displaying a half‐wave potential of 0.89 V vs RHE and 0.74 V vs RHE under alkaline (0.1 m KOH) and acidic (0.1 m HClO 4 ) media, respectively, thanks to the balanced * OOH intermediate adsorption and desorption induced by the pentagonal carbon topological defects and nitrogen dopants. The aqueous zinc‐air battery (ZAB) equipped with the NCA‐Cl cathode delivers a peak power density of 206.6 mW cm −2 , a specific capacity of 810.6 mAh g −1 , and a durability of 400 h, and the flexible ZAB also performed convincingly. This work provides an effective strategy for the formation of topological carbon defects for the enhancement of the electrocatalytic activity of carbon‐based catalysts.