Electrostatic‐Attraction‐Driven Self‐Assembled Graphene‐Disordered Rocksalt Composite Cathode for Lithium‐Ion Batteries

ABSTRACT Disordered rocksalt cathodes hold promise for achieving high‐capacity lithium‐ion batteries while using low‐cost, earth‐abundant elements. However, their electrochemical performance remains critically limited by their poor electronic conductivity. Conventional strategies such as high‐energy ball milling with excess carbon additives can improve conductivity but remain challenging to scale and often produce defects and increase surface area, thereby accelerating capacity degradation. Herein, we report an alternative approach of electrostatic‐attraction‐driven self‐assembly to fabricate Li _1.2 Mn _0.6 Ti _0.2 O _1.8 F _0.2 (LMTOF) particles uniformly wrapped with electronically conductive graphene sheets without associated materials degradation. The graphene‐wrapped LMTOF demonstrates significantly improved cycling stability (89% capacity retention after 100 cycles) and superior rate capability compared with an LMTOF‐carbon composite electrode fabricated using the conventional high‐energy ball‐milling process. Post‐cycling analysis reveals reduced oxygen evolution, suppressed unwanted side reactions, and improved structural integrity for the graphene‐LMTOF composite. This work highlights the advantages of solution‐based carbon wrapping and offers a scalable strategy to prepare high‐performance DRX cathodes for lithium‐ion batteries.