High‐Performance Poly(1‐naphthylamine)/Mesoporous Carbon Cathode for Lithium‐Ion Batteries with Ultralong Cycle Life of 45000 Cycles at ‐15 °C

Abstract Organic electrode materials for lithium‐ion batteries have attracted significant attention in recent years. Polymer electrode materials, as compared to small‐molecule electrode materials, have the advantage of poor solubility, which is beneficial for achieving high cycling stability. However, the severe entanglement of polymer chains often leads to difficulties in preparing nanostructured polymer electrodes, which is vital for achieving fast reaction kinetics and high utilization of active sites. This study demonstrates that these problems can be solved by the in situ electropolymerization of electrochemically active monomers in nanopores of ordered mesoporous carbon (CMK‐3), combining the advantages of the nano‐dispersion and nano‐confinement effects of CMK‐3 and the insolubility of the polymer materials. The as‐prepared nanostructured poly(1‐naphthylamine)/CMK‐3 cathode exhibits a high active site utilization of 93.7%, ultrafast rate capability of 60 A g −1 (≈320 C), and an ultralong cycle life of 10000 cycles at room temperature and 45000 cycles at −15 °C. The study herein provides a facile and effective method that can simultaneously solve both the dissolution problem of small‐molecule electrode materials and the inhomogeneous dispersion issue of polymer electrode materials.