Redox-active organic materials have emerged as promising alternatives to conventional inorganic electrode materials for battery energy storage owing to their high capacity, environmental friendliness and sustainability. However, organic electrode materials in practical devices suffer from poor cycling stability due to their undesired solubility in electrolyte solvents, sluggish charge transfer and mass transport, as well as processing complexity. Microporous materials with ordered nanopores have emerged as promising electrode materials for metal-ion batteries. However, the processing and fabrication of these materials into electrodes remain challenging. Here, I will present a new molecular engineering approach to redox-active polymers of intrinsic microporosity (PIMs) that possess an open network of sub-nanometer pores and abundant accessible carbonyl-based redox sites for fast lithium-ion transport and storage. The redox-active PIMs can be solution-processed into thin films and polymer-carbon composites with a homogeneously dispersed microstructure, while remaining insoluble in electrolyte solvents. Solution-processed electrodes demonstrate improved cycling performance in lithium-ion batteries with high capacity retention. Redox-active PIMs that combine intrinsic microporosity, reversible redox activity with solution processability may have broad utility in a variety of electrochemical devices for energy storage, sensors and electronic applications.

Solution-processable redox-active polymers of intrinsic microporosity for electrochemical energy storage

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ACS Fall 2022

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