Solution-Processable Redox-Active Polymers of Intrinsic Microporosity for Electrochemical Energy Storage
Anqi Wang, Rui Tan, Charlotte Breakwell, Xiaochu Wei, Zhiyu Fan, Chunchun Ye, Richard Malpass‐Evans, Tao Liu, Martijn A. Zwijnenburg, Kim E. Jelfs, Neil B. McKeown, Jun Chen, Qilei Song
Abstract
Redox-active organic materials have emerged as promising alternatives to conventional inorganic electrode materials in electrochemical devices for energy storage. However, the deployment of redox-active organic materials in practical lithium-ion battery devices is hindered by their undesired solubility in electrolyte solvents, sluggish charge transfer and mass transport, as well as processing complexity. Here, we report a new molecular engineering approach to prepare redox-active polymers of intrinsic microporosity (PIMs) that possess an open network of subnanometer pores and abundant accessible carbonyl-based redox sites for fast lithium-ion transport and storage. 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 redox-active PIM electrodes demonstrate improved cycling performance in lithium-ion batteries with no apparent capacity decay. Redox-active PIMs with combined properties of intrinsic microporosity, reversible redox activity, and solution processability may have broad utility in a variety of electrochemical devices for energy storage, sensors, and electronic applications.