Covalent organic frameworks (COFs) have attracted growing interest by virtue of their structural diversity and tunability. Herein, we present a novel approach for the development of organic rechargeable battery cathodes in which three distinct redox-active COFs were successfully prepared and delaminated into 2D few-layer nanosheets. Compared with the pristine COFs, the exfoliated COFs with shorter Li diffusion pathways allow a significant higher utilization efficiency of redox sites and faster kinetics for lithium storage. Unlike diffusion-controlled manners in the bulk COFs, the redox reactions in ECOFs are mainly dominated by charge transfer process. The capacity and potential are further engineered by reticular design of COFs without altering the underlying topology. Specifically, DAAQ-ECOF exhibits excellent rechargeability (98% capacity retention after 1800 cycles) and fast charge-discharge ability (74% retention at 500 mA g as compared to at 20 mA g). DABQ-ECOF shows a specific capacity of 210 mA h g and a voltage plateau of 2.8 V.

Covalent organic frameworks (COFs) with well-tailored channels are able to accommodate ions and offer their conduction pathway. However, due to strong Coulombic interaction and the lack of transport medium, directly including lithium salts into the channels of COFs results in limited ion transport capability. Herein, we propose a strategy of incorporating low-molecular-weight polyethylene glycol (PEG) into COFs with anionic, neutral, or cationic skeletons to accelerate Li+ conduction. The PEG confined in the well-aligned channels retains high flexibility and Li+ solvating ability. The ion conductivity of PEG included in a cationic COF can reach 1.78 × 10–3 S cm–1 at 120 °C. The simplicity of this strategy as well as the diversity of crystalline porous materials holds great promise to design high-performance all-solid-state ion conductors.

Covalent organic frameworks with hydroxy groups in the pore wall, which exhibit efficient, metal-free, heterogeneous catalytic performances for chemical fixation of CO2 under mild conditions, are reported.

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