aromatic groups, which via columnar π-π stacking order into a periodic 3D structure (Scheme S1, Supporting Information). Their modular construct and ordered porosity makes them find use in diverse applications Here we are seeking application of 2D COFs in metal-ion batteries, which are typically made of electrodes with layered structures, for example, graphite as anode and LiCoO 2 as cathode. Owing to their graphite resembling structure, COF can serve as anode. Since their initial discovery, many 2D materials with comparable layered structures have been explored as lithium insertion-deinsertion materials. [28][29][30][31][32][33][34][35][36][37][38][39] Some of the highly desirable characteristics of a superior anode material include moderate to high surface accessibility to ensure maximum charge storage per unit area, and the other is the hierarchical porosity for favorable kinetics. Exfoliation enhances surface accessibility and active site creation in such 2D materials. [40][41][42][43][44][45][46][47][48] In this regard, COFs could have much more to offer. [49][50][51] Exfoliation in any 2D material is largely dependent on the interlayer forces holding them. Typically, the COF layers are held together by interlayer π-π interactions or in some cases via additional hydrogen bonding. [52,53] However, unlike graphite, the layers of COF are not built from fused aromatic rings. In their optimized Covalent organic framework (COF) can grow into self-exfoliated nanosheets. Their graphene/graphite resembling microtexture and nanostructure suits electrochemical applications. Here, covalent organic nanosheets (CON) with nanopores lined with triazole and phloroglucinol units, neither of which binds lithium strongly, and its potential as an anode in Li-ion battery are presented. Their fibrous texture enables facile amalgamation as a coin-cell anode, which exhibits exceptionally high specific capacity of ≈720 mA h g −1 (@100 mA g −1 ). Its capacity is retained even after 1000 cycles. Increasing the current density from 100 mA g −1 to 1 A g −1 causes the specific capacity to drop only by 20%, which is the lowest among all high-performing anodic COFs. The majority of the lithium insertion follows an ultrafast diffusion-controlled intercalation (diffusion coefficient, D Li + = 5.48 × 10 −11 cm 2 s −1 ). The absence of strong Liframework bonds in the density functional theory (DFT) optimized structure supports this reversible intercalation. The discrete monomer of the CON shows a specific capacity of only 140 mA h g −1 @50 mA g −1 and no sign of lithium intercalation reveals the crucial role played by the polymeric structure of the CON in this intercalation-assisted conductivity. The potentials mapped using DFT suggest a substantial electronic driving-force for the lithium intercalation. The findings underscore the potential of the designer CON as anode material for Li-ion batteries.
Lithium Storage