Anchored Oxygen-Release-Suppression Phase Stabilizing High-Voltage Ni-Rich Cathode Materials

The Ni-rich LiNi_xCo_yMn_1-x-yO₂ (x ≥ 0.9) cathode materials (NCMs) have been considered promising for next-generation Li-ion batteries owing to their high-energy density. However, their practical application is hindered by gas evolution and rapid capacity degradation, primarily caused by irreversible oxygen release and structural instability. Herein, a facile one-step anchoring strategy is proposed to overcome this challenge by engineering a precisely tailored dual-architecture LiNi_0.9Co_0.05Mn_0.05O₂ (DA-NCM). This strategy constructs a dual-phase surface architecture on Ni-rich cathodes, where perovskite-phase La₄LiNiO₈ mitigates surface oxygen instability and interfacial degradation, and inert La₂Mo₂O₉ anchors the lattice to avoid the detachment of La₄LiNiO₈ during cycling via enhanced La─O bond pinning effect. This dual-architecture design provides a robust strategy for stabilizing the interface, surface, and bulk phase of Ni-rich cathodes, enabling durable oxygen regulation, suppressed structural degradation, and stable high-voltage operation under demanding cycling conditions. Thus, our DA-NCM cathodes demonstrate excellent capacity retention of 95.7% at 4.3 V and 93.6% at 4.5 V after 200 cycles and remarkable stability even at an elevated temperature (50°C) and high voltage (4.5 V), confirming their markedly enhanced electrochemical stability. This precision design of dual architecture provides a new pathway for developing high-energy-density cathode materials with long cycle life.