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Isometric Covalent Triazine Frameworks Derived Porous Carbons as Efficient Metal‐Free Electrocatalysts for Oxygen Reduction Reactions

Covalent triazine frameworks (CTFs) and their derived N-doped carbons have attracted tremendous attention due to their wide application in energy conversion and storage in the past few years. However, previous interests mainly focused on development of new building blocks and optimizing the synthetic conditions. Taking advantage of the isometric building blocks to control the porous structure and to fundamentally understand the structure-property relationship are rarely reported. In this work, two isometric building blocks are used to produce isometric CTFs with controllable pore geometries. As-prepared CTF with non-planar hexagonal pores demonstrates higher surface area, larger pore volume and richer N content in comparison with the planar CTF. After pyrolysis, corresponding N-doped carbons derived from non-planar porous CTF at 900 oC exhibit admirable catalytic activity for oxygen reduction in alkaline media (half-wave potential: 0.86 V; Tafel slope: 65 mV dec-1), owing to the larger pore volume together with rich pyridinic and quaternary N species. When assembled into a zinc-air battery, as-made electrocatalysts show high capacity up to 651 mAh g-1 and excellent durability. This work design two kinds of tailoring and scalable CTFs and their-derived porous carbons material, which are highly efficient electrocatalysts for energy conversion and storage.

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