Solvent‐Free Synthesis of Covalent Organic Framework/Graphene Nanohybrids: High‐Performance Faradaic Cathodes for Supercapacitors and Hybrid Capacitive Deionization

Abstract Covalent organic frameworks (COFs) with flexible periodic skeletons and ordered nanoporous structures have attracted much attention as potential candidate electrode materials for green energy storage and efficient seawater desalination. Further improving the intrinsic electronic conductivity and releasing porosity of COF‐based materials is a necessary strategy to improve their electrochemical performance. Herein, the employed graphene as the conductive substrate to in situ grow 2D redox‐active COF (TFPDQ‐COF) with redox activity under solvent‐free conditions to prepare TFPDQ‐COF/graphene (TFPDQGO) nanohybrids and explores their application in both supercapacitor and hybrid capacitive deionization (HCDI). By optimizing the hybridization ratio, TFPDQGO exhibits a large specific capacitance of 429.0 F g −1 due to the synergistic effect of the charge transport highway provided by the graphene layers and the abundant redox‐active centers contained in the COF skeleton, and the assembled TFPDQGO//activated carbon (AC) asymmetric supercapacitor possesses a high energy output of 59.4 Wh kg −1 at a power density of 950 W kg −1 and good cycling life. Furthermore, the maximum salt adsorption capacity (SAC) of 58.4 mg g −1 and stable regeneration performance is attained for TFPDQGO‐based HCDI. This study highlights the new opportunities of COF‐based hybrid materials acting as high‐performance supercapacitor and HCDI electrode materials.