• • The low-nickel cathode Li(Li0.05Ni0.57Mn0.31Co0.07)O2 (Ni<60%) achieves high discharge capacity and cycling stability comparable to Ni-rich cathodes (N80/N90), reducing nickel content by over 20% and mitigating supply chain risks.
• • mRIXS analysis reveals a persistent spectral feature at 4.5 V, indicating highly reversible lattice oxygen redox that remains largely unchanged after 100 cycles, directly contributing to capacity retention.
• • The radially integrated structure comprises three phases: an outermost rock-salt phase with lithium-percolation channels, an intermediate Li/Mn-rich phase with delocalized superlattice ordering, and an inner Ni-rich layered phase, enabling synergistic '1+1+1>3' performance.
• • In-situ high-energy X-ray diffraction demonstrates minimized lattice variations and suppressed Ni oxidation state changes during cycling, addressing bulk structural degradation and interfacial side reactions.