A covalent organic framework with asymmetric coordination for the oxygen reduction reaction: a computational study

Abstract

Through constant-potential first-principles calculations coupled with microkinetic modelling, a covalent organic framework with an asymmetric CoN₂O₂ moiety is identified to exhibit remarkable oxygen reduction activity, for which the theoretical half-wave potential is 0.98 V. Electronic structure analysis reveals that the asymmetric coordination environment effectively modulates charge redistribution at the active site, thereby enhancing the activation of oxygen species.