In Situ Electropolymerization Enables Ultrafast Long Cycle Life and High‐Voltage Organic Cathodes for Lithium Batteries

Abstract Organic cathode materials have attracted extensive attention because of their diverse structures, facile synthesis, and environmental friendliness. However, they often suffer from insufficient cycling stability caused by the dissolution problem, poor rate performance, and low voltages. An in situ electropolymerization method was developed to stabilize and enhance organic cathodes for lithium batteries. 4,4′,4′′‐Tris(carbazol‐9‐yl)‐triphenylamine (TCTA) was employed because carbazole groups can be polymerized under an electric field and they may serve as high‐voltage redox‐active centers. The electropolymerized TCTA electrodes demonstrated excellent electrochemical performance with a high discharge voltage of 3.95 V, ultrafast rate capability of 20 A g −1 , and a long cycle life of 5000 cycles. Our findings provide a new strategy to address the dissolution issue and they explore the molecular design of organic electrode materials for use in rechargeable batteries.