Unlocking the Charge-Storage Potential of a Phenanthraquinone-based Two-Dimensional Covalent Organic Framework (2D COF).

The high surface area, open pore-structure and atomic-level organization inherent in many covalent organic frameworks (COFs) make them an attractive polymer platform for developing functional materials. Herein, a chemically robust 2D COF (TpOMe-DAPQ COF) containing phenanthraquinone moieties was prepared by condensing 2,4,6-trimethoxy-1,3,5-benzenetricarbaldehyde (TpOMe) and 2,7-diamino-9,10-phenanthraquinone (DAPQ) using the convenient mechanochemical method. The poor charge-storage capacity of the pristine TpOMe-DAPQ COF was substantially improved by first investigating its redox-site accessibility (RSA) using different conductivity-enhancement methods, and then optimizing the amount of EDOT needed to perform an in-situ polymerization. The resulting composite (0.4EDOT@TpOMe-DAPQ) was characterized and its enhanced charge-storage capabilities enabled it to be used as an anode material in an aqueous Mn beaker-cell battery capable of delivering 0.76 V. This work outlines the rational design approach used to develop a functional charge-storage material utilizing a COF-based polymerization platform.