Chemical Exfoliation as a Controlled Route to Enhance the Anodic Performance of COF in LIB

Abstract A covalent organic framework (COF), built from light atoms with a graphitic structure, could be an excellent anodic candidate for lightweight batteries, which can be of use in portable devices. But to replace the commercial graphite anode, they need more Li‐interactive sites/unit‐cell and all such sites should be made to participate. The compromise made in the volumetric density to gain the gravimetric advantage should be minimal. Exfoliation enhances surface/functional group accessibility yielding high capacity and rapid charge storage. A chemical strategy for simultaneous exfoliation and increase of Li‐loving active‐pockets can deliver a lightweight Li‐ion battery (LIB). Here, anthracene‐based COFs are chemically exfoliated into few‐layer‐thick nanosheets using maleic anhydride as a functionalizing exfoliation agent. It not only exfoliates but also introduces multiple Li‐interactive carbonyl groups, leading to a loading of 30 Li/unit‐cell (vs one Li per C 6 ). The exfoliation enhances the specific capacity by ≈4 times (200–790 mAh g −1 @100 mA g −1 ). A realistic full‐cell, made using the exfoliated COF against a LiCoO 2 cathode, delivers a specific capacity of 220 mAh g −1 over 200 cycles. The observed capacity stands highest among all organic polymers. For the first report of a COF derived full‐cell LIB, this is a windfall.