Anchoring Nickel and Stabilizing Oxygen in Coherent LiNiO<sub>2</sub>@LiFePO<sub>4</sub> Composite Cathode Materials for Rechargeable Lithium-Ion Batteries.

Hou, Zhichen; Wang, Wanying; Yao, Meng; Liu, Kuiming; Kong, Fanqi; Huang, Xinhui; Li, Yue; Ding, Guoyu et al. · Adv Mater · 2025

basic_science · Level V

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Abstract

LiNiO<sub>2</sub> is an appealing cathode material for Li-ion batteries because of high energy density and low cost but suffers from irreversible phase transition and surface instability. Herein, a ball-milled LiNiO<sub>2</sub>@LiFePO<sub>4</sub> composite with oriented coherent combination is reported with enhanced structural stability and Li<sup>+</sup> diffusion. The coherent oriented channels are demonstrated to favor the reversible and rapid Li<sup>+</sup> intercalation during the H2-H3 phase transition, which significantly alleviates structural strain accumulation. The covalent P─O bonds anchored on the LiNiO<sub>2</sub> surface stabilizes the Ni sites, mitigating surface reconstruction and lattice oxygen loss. The LiNiO<sub>2</sub>@LiFePO<sub>4</sub> cathode exhibits a specific capacity of 210 mAh g<sup>-1</sup> and an initial Coulombic efficiency of 93.7% at 0.1 C, along with a remarkable rate capability of 156 mAh g<sup>-1</sup> at 10 C. Furthermore, the full cells pairing LiNiO<sub>2</sub>@LiFePO<sub>4</sub> cathode and graphite anode deliver a considerable energy density over 280 Wh kg<sup>-1</sup> and a remarkable capacity retention. This study offers an effective approach of phosphate coalesce to upgrade high-capacity nickel-rich oxide cathode materials.