Abstract

A covalent organic framework that is composed of hexachlorocyclotriphosphazene and dicyanamide has been coated on CNT to prepare metal-free oxygen reduction reaction catalyst through thermal polymerization of the Zn-air battery cathode. The N,P-codoped nanohybrids have highly porous structure and active synergistic effect between graphitic-N and -P, which promoted the electrocatalytic performance. The electrocatalysts exhibits remarkable half-wave potential (-0.162 V), high current density (6.1 mA/cm-2), good stability (83%), and excellent methanol tolerance for ORR in alkaline solution. Furthermore, the N,P-codoped nanohybrids were used as an air electrode for fabrication of a high performance Zn-air battery. The battery achieves a high open-circuit potential (1.53 V) and peak power density (0.255 W cm-2). Moreover, the effect of N,P codoping on the conjugate carbon system and the synergistic effect between graphitic-N and P have been calculated through density functional theory calculations, which are essentially in agreement with experimental data.

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