Molecular engineering regulation redox‐dual‐active‐center covalent organic frameworks‐based anode for high‐performance Li storage

Abstract Covalent organic frameworks (COFs) show considerable attention and potential value in energy storage and conversion. However, design and preparation novel dual‐active‐center modified COFs for high‐performance Li storage and accelerating Li diffusion are still challengeable. In this work, we synthesize dual‐active‐group of CN and CO decorated COF (denoted as Tp‐Ta‐COF) as the anode material for lithium‐ion batteries (LIBs). Benefiting from the dual‐active‐site, the Li + diffusion kinetics on the Tp‐Ta‐COF are improved and Tp‐Ta‐COF electrode delivers high reversible capacity of 413 mAh g −1 under current density with 200 mA g −1 . Moreover, 18 Li + can be embed in Tp‐Ta‐COF with CN and CO containers. The mechanism between Li + and active‐site is deeply deduced and studied by multiple in situ techniques and density functional theory (DFT) theoretical calculation, suggesting interactions of Li + and active‐group are highly reversible procedures. Consequently, we expect this work could create a universal strategy for construction high‐performance Li storage COF‐based materials. image