Mesoporous Polyimide-Linked Covalent Organic Framework with Multiple Redox-Active Sites for High-Performance Cathodic Li Storage

Covalent organic frameworks (COFs) are gaining increasing attention as renewable cathode materials for Li-ion batteries. However, COF electrodes reported so far still exhibit unsatisfying capacity due to their limited active site density and insufficient utilization. Herein, a new two-dimensional polyimide-linked COF, HATN-AQ-COF with multiple redox-active sites for storing Li+ ions, was designed and fabricated from a new module of 2,3,8,9,14,15-hexacarboxyl hexaazatrinaphthalene trianhydrides with a 2,6-diaminoanthraquinone linker. HATN-AQ-COF possessing excellent stability, good conductivity, and a large pore size of 3.8 nm enables the stable and fast ion transport. This, in combination with the abundant redox active sites, results in a high reversible capacity of 319 mAh g(-1) at 0.5 C (1 C=358 mA g(-1)) for the HATN-AQ-COF electrode with a high active site utilization of 89 % and good cycle performance, representing one of the best performances among the reported COF electrodes.

Automated summary

Covalent organic frameworks (COFs) have gained attention as promising cathode materials for Li-ion batteries. However, the capacity of COF electrodes reported so far is still unsatisfactory. In this study, a new two-dimensional polyimide-linked COF, HATN-AQ-COF, was designed and fabricated. It possesses multiple redox-active sites for Li+ ion storage, excellent stability, good conductivity, and a large pore size. The HATN-AQ-COF electrode demonstrates a high reversible capacity, active site utilization, and cycle performance, making it one of the best performers among reported COF electrodes.