COF-Based Electrodes with Vertically Supported Tentacle Array for Ultrahigh Stability Flexible Energy Storage

As an emerging porous crystal polymer, covalent organic frameworks (COFs) possess unique characteristics, such as high porosity, excellent stability, diverse topologies, designable open channels, and functional tunability. However, limited by the solid powder form, most COFs display low active site utilization and weak binding force with the current collector. In this pioneering research, we integrate redox-active COFs onto carbon fiber surfaces (AC-COFs) via strong covalent bridging. The 2,6-diaminoanthraquinone (DAAQ) pillars embedded on the carbon fiber surface are the key to precisely controlling the growth direction of COFs. The obtained tentacle-like array vertically supported on the surface of the carbon fiber can effectively induce charge transfer and prevent COFs from aggregating/collapsing. The strong covalent coupling and increase of accessible active sites contributed to the high specific capacitance of AC-COFs electrode (1034 mF cm–2). In addition, the COF-based flexible electrode retains an initial capacitance of 98% after 20000 charge–discharge cycles. The flexible all-solid-state symmetric supercapacitor is assembled by PVA/H2SO4 gel electrolyte with an areal capacitance of 715 mF cm–2. Besides, a red LED can be easily powered by three-bending AC-COFs//AC-COFs devices. The innovative synthesis strategy opens up new opportunities to develop high-performance flexible energy storage devices based on COFs.