Ultrastable Triazine-Based Covalent Organic Framework with an Interlayer Hydrogen Bonding for Supercapacitor Applications

Covalent organic frameworks (COFs) with redox-active units are a class of ideal materials for electrochemical-energy-storage devices. A novel two-dimensional (2D) PDC-MA-COF with redox-active triazine units was prepared via aldehyde-amine condensation reaction by using 1,4-piperazinedicarboxaldehyde (PDC) and melamine (MA) as structural units, which possessed high specific surface area (SBET = 748.2 m2 g-1), narrow pore width (1.9 nm), large pore volume (1.21 cm3 g-1), and high nitrogen content (47.87%), for pseudocapacitance application. The interlayer C-H···N hydrogen bonding can "lock" the relative distance between two adjacent layers to avoid an interlayer slip, which is more conducive to maintaining the ordered pore structure of the COF and improving a fast charge transfer between the electrode interface and triazine units. The PDC-MA-COF exhibited an excellent electrochemical performance with the highest specific capacitance of 335 F g-1 along with 19.71% accessibility of the redox-active triazine units in a three-electrode system and 94 F g-1 in a two-electrode system at 1.0 A g-1 current density. Asymmetric supercapacitor of PDC-MA-COF//AC assembled using PDC-MA-COF and activated carbon (AC) as positive and negative electrode materials, respectively, exhibited a high energy density of 29.2 W h kg-1 with a power density of 750 W kg-1. At the same time, it also showed an excellent cyclic stability and could retain 88% of the initial capacitance after 20 000 charge-discharge cycles, which was better than those of the most of the analogous materials reported previously. This study provided a new strategy for designing redox-active COFs for pseudocapacitive storage.