Boosting supercapacitive performance of pristine covalent organic frameworks via phenolic hydroxyl groups: A...

Two-dimensional covalent organic frameworks (COFs) are ideal electrode materials for electrochemical energy storage devices due to their unique structures and properties, and the accessibility and utilization efficiency of the redox-active sites within COFs are critical determinants of their pseudocapacitive performance. Via introducing meticulously designed phenolic hydroxyl (Ar-OH) groups with hydrogen-bond forming ability onto the imine COF skeletons, DHBD-Sb-COF exhibited improved hydrophilicity and crystallinity than the parent BD-Sb-COF, the redox-active sites (SbPh₃ moieties) in COF electrodes could thus be highly accessed by aqueous electrolyte with a high active-site utilization of 93%. DHBD-Sb-COF//AC provided an excellent supercapacitive performance with an energy density of 78 Wh Kg^-1 at the power density of 2553 W Kg^-1 and super cycling stability, exceeding most of the previously reported pristine COF electrode-based supercapacitors. The "two-in-one" strategy of introducing hydroxyl groups onto imine COF skeletons to enhance both hydrophilicity and crystallinity provides a new avenue to improve the electrochemical performance of COF-based electrodes for high-performance supercapacitors.