Exceptional Sodium-Ion Storage by an Aza-Covalent Organic Framework for High Energy and Power Density Sodium-Ion Batteries

Redox-active covalent organic frameworks (COFs) are a new class of material with the potential to transform electrochemical energy storage due to the well-defined porosity and readily accessible redox-active sites of COFs. However, combining both high specific capacity and energy density in COF-based batteries remains a considerable challenge. Herein, we demonstrate the exceptional performance of Aza-COF in rechargeable sodium-ion batteries (SIBs). Aza-COF is a microporous 2D COF synthesized from hexaketocyclohexane and 1,2,4,5-benzenetetramine by a condensation reaction, which affords phenazine-decorated channels and a theoretical specific capacity of 603 mA h g^-1. The Aza-COF-based electrode exhibits an exceptional average specific capacity (550 mA h g^-1), energy density (492 W h kg^-1) at 0.1 C, and power density (1182 W kg^-1) at 40 C. The high capacity and energy density are attributed to swift surface-controlled redox processes and rapid sodium-ion diffusion inside the porous electrode. Rate capability studies showed that the battery also performs well at high current rates: 1 C (363 mA h g^-1), 5 C (232 mA h g^-1), 10 C (161 mA h g^-1), and 20 C (103 mA h g^-1). In addition, the long-term cycling stability test revealed very good capacity retention (87% at 5 C) and Coulombic efficiencies near unity over 500 cycles.