Edge-on-Plane-Confined Covalent Organic Frameworks Enable a Defect- and Nitrogen-Rich Carbon Matrix for High-Rate Lithium-Ion Storage

Nitrogen-rich layered carbon could be an eligible anode material for high-performance lithium-ion batteries (LIBs) thanks to their enriched reactive sites and fast kinetics of ion transportation. Covalent organic frameworks (COFs) provide promising parental sources for the fabrication of N-rich layered carbon, but the controllable synthesis of COFs remains challenging. Herein, a confined COF nanosheet array is anchored on functionalized graphene in an edge-on-plane orientation through a successive covalent binding process. The covalently bonded hybrid material is derived from a highly porous (specific surface area, 1093 m 2 g –1 ), defect- and N-rich (11 atom %) carbon matrix (NCM) through pyrolysis. The as-obtained NCM as an anode in LIBs exhibits high capacity (1162 mA h g –1 at 0.1 A g –1 ), good rate performance (270 mA h g –1 at 10 A g –1 ), and cycling stability (345 mA h g –1 at 5 A g –1 after 400 cycles). The successive covalent binding manipulation for the confined and oriented growth of COFs would inspire more prudent COF nanostructures for electrochemical energy storage.