Isometric Covalent Triazine Framework‐Derived Porous Carbons as Metal‐Free Electrocatalysts for the Oxygen Reduction Reaction

Abstract Covalent triazine frameworks (CTFs) and their derivative N‐doped carbons have attracted much attention for application in energy conversion and storage. However, previous studies have mainly focused on developing new building blocks and optimizing synthetic conditions. The use of isometric building blocks to control the porous structure and to fundamentally understand structure–property relationships have rarely been reported. In this work, two isometric building blocks are used to produce isometric CTFs with controllable pore geometries. The as‐prepared CTF with nonplanar hexagonal rings demonstrates higher surface area, larger pore volume, and richer N content than the planar CTF. After pyrolysis, nonplanar porous CTF‐derived N‐doped carbons exhibit admirable catalytic activity for oxygen reduction in alkaline media (half‐wave potential: 0.86 V; Tafel slope: 65 mV dec −1 ), owing to their larger pore volume and the abundance of pyridinic and graphitic N species. When assembled into a zinc–air battery, the as‐made electrocatalysts show high capacities of up to 651 mAh g −1 and excellent durability.