Weak Intermolecular Interactions in Covalent Organic Framework-Carbon Nanofiber Based Crystalline yet Flexible Devices.

The redox-active and porous structural backbone of covalent organic frameworks (COFs) can facilitate high-performance electrochemical energy storage devices. However, the utilities of such 2D materials as supercapacitor electrodes in advanced self-charging power-pack systems have been obstructed due to the poor electrical conductivity and subsequent indigent performance. Herein, we report an effective strategy to enhance the electrical conductivity of COF thin sheets through the in situ solid-state inclusion of carbon nanofibers (CNF) into the COF precursor matrix. The obtained COF-CNF hybrids possess a significant intermolecular π···π interaction between COF and the graphene layers of the CNF. As a result, these COF-CNF hybrids (DqTp-CNF and DqDaTp-CNF) exhibit good electrical conductivity (0.25 × 10 S cm), as well as high performance in electrochemical energy storage (DqTp-CNF: 464 mF cm at 0.25 mA cm). Also, the fabricated, mechanically strong quasi-solid-state supercapacitor (DqDaTp-CNF SC) delivered an ultrahigh device capacitance of 167 mF cm at 0.5 mA cm. Furthermore, we integrated a monolithic photovoltaic self-charging power pack by assembling DqDaTp-CNF SC with a perovskite solar cell. The fabricated self-charging power pack delivered excellent performance in the areal capacitance (42 mF cm) at 0.25 mA cm after photocharging for 300 s.