Interwoven Phase Stabilization in Ni-Rich Cathode Material via Nanoparticle-Seeded Synthesis

Nickel-rich (Ni-rich) layered oxides offer high specific capacities but suffer from rapid degradation during prolonged cycling, with anisotropic lattice deformation being a widely discussed cause. Embedding strain-buffering phases within the cathode structure mitigates this degradation by suppressing adverse volumetric changes. Here, a flame-assisted spray pyrolysis method is developed to introduce interwoven rocksalt-like and spinel-like phases into layered structured Li(Ni 0.8 Co 0.1 Mn 0.1 )O 2 (NCM811) using nanoparticle-laden suspension precursors containing nickel hydroxide. Electrochemical measurements and in situ X-ray diffraction demonstrated enhanced structural stability during cycling. Atomic-resolution HAADF-STEM imaging reveals that the secondary phases form coherent, interwoven nanoscale domains within the primary layered matrix. This rapid and scalable synthesis approach enables heterogeneous phase engineering in Ni-rich cathodes, offering a viable route toward improved cycling stability. The results underscore the potential of nanoparticle-seeded precursors for tailoring the phase architecture in energy materials.