Covalent Organic Frameworks as Model Materials for Fundamental and Mechanistic Understanding of Organic Battery Design Principles

[Image: see text] Redox-active covalent organic frameworks (COFs) have recently emerged as advanced electrodes in polymer batteries. COFs provide ideal molecular precision for understanding redox mechanisms and increasing the theoretical charge-storage capacities. Furthermore, the functional groups on the pore surface of COFs provide highly ordered and easily accessible interaction sites, which can be modeled to establish a synergy between ex situ/in situ mechanism studies and computational methods, permitting the creation of predesigned structure–property relationships. This perspective integrates and categorizes the redox functionalities of COFs, providing a deeper understanding of the mechanistic investigation of guest ion interactions in batteries. Additionally, it highlights the tunable electronic and structural properties that influence the activation of redox reactions in this promising organic electrode material.