One‐Pot Spray Pyrolysis Fabrication of Multi‐Phase Lithium Manganese Oxide Microsphere Cathodes for Enhanced Lithium‐Ion Battery Performance

Spinel‐type lithium manganese oxide (LMO) cathodes offer low cost, environmental benignity, and strong thermal safety, making them attractive for fast‐charge lithium‐ion batteries. Their widespread adoption, however, has been hindered by structural degradation associated with the Jahn–Teller distortion of Mn 3+ . Here, we report for the first time a rapid, single‐step spray pyrolysis route that produces multi‐phase microspheres comprising Sr‐doped LiMn 2 O 4 spinel, a minor Sr 2 Mn 2 O 5 phase, and a C2/m layered Li 2 MnO 3 ‐like structure, all crystallized directly from a single precursor solution without post‐treatment. This continuous aerosol process enables uniform Sr incorporation, precise morphological control, and manufacturing scalability. The synergistic coexistence of these phases provides multiple benefits: Sr doping lowers the Mn 3+ fraction, suppresses lattice distortion, and stabilizes the spinel framework; the Sr 2 Mn 2 O 5 phase refines particle morphology and mitigates mechanical stress during cycling; and the layered Li 2 MnO 3 ‐like domains enhance structural stability, diversify Li + diffusion pathways, and suppress Mn dissolution and electrolyte side reactions. As a result, the composite cathode delivers improved electrochemical performance, retaining 81.72 mA h g −1 after 400 cycles at 1 C and 76.78 mA h g −1 at 5 C, demonstrating that rapid, single‐step spray pyrolysis is an effective and scalable strategy for robust, high‐voltage spinel cathodes.