Covalent Organic Frameworks (COFs) represent crystalline organic polymers with permanent porosity. They can have pi-stacked layered structures, which can be exfoliated. This can improve their surface accessibility and diffusion, leaving a marked impact on their host-guest interactions. Here, we present a designed strategy that exfoliates two imide-based COFs into few-layer-thick nanosheets. We introduce the concept of “Functionalizing Exfoliation Agent (FEA)” in our strategy. The FEA not only exfoliates the polymeric COF into few-layer thick nanosheets, but it simultaneously functionalizes the COF with an increased number of guest-binding groups. Their covalent linking to the COF without altering the polymeric structure means permanent incorporation of functional groups and no leaching. As a proof-of-concept, we demonstrate that a specific FEA attached to COFs (IISERP-COF7 and IISERP-COF8) exfoliates them to covalent organic nanosheets that show four times (200 mAh/g to 790 mAh/g @ 100 mA/g) enhancement in anodic characteristics when employed in a Li-ion battery. Moreover, a practical full-cell made using the resorcinol-derived CON anode against LiCoO2 cathode, delivers a stable specific capacity of 220 mAh/g @ 100mA/g with an energy density of 364Wh/kg (vs. 320Wh/kg for graphite). The CON retains 92% of its performance over 200 cycles; the commercial graphite with an initial full-cell capacity of 220 mAh/g drops to 170 mAh/g after 200 cycles. The observed full-cell capacity stands highest among all organic-polymers operating with lithium insertion or intercalation type phenomenon. To the extent of our knowledge, for the first report of a full-cell performance of a COF-derived LIB, this is a windfall.

Redox-active covalent organic frameworks as anodes in LIB

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.