Mitigating Surface Lithium Silting via Coherent Lattice Anchoring to Stabilize LiNiO2 Cathode Materials

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Abstract Layered LiNiO2 (LNO) is a promising cathode material for high-energy-density lithium-ion batteries but is limited by rapid capacity fade on electrochemical cycling. While the structural instability of LNO is well-recognized to correlate with oxygen loss and cation mixing, the impact of sluggish ionic transport on performance degradation remains underexplored. Here, we identify lithium silting—localized near-surface Li enrichment in charged LNO particles—as an early-stage degradation feature associated with local stress accumulation, dislocation formation, and subsequent structural degradation. To address this issue, we develop a lattice anchoring strategy by simultaneous Zr doping and constructing a nanoscale La4[LiNi]O8 coating layer with crystallographic coherence to the LNO phase. The bulk Zr doping stabilizes the lattice while the coherent interface preserves structural integrity and continuous ionic transport pathways to effectively suppress the surface lithium silting. The modified LNO with Zr doping and La4[LiNi]O8 coating exhibits significantly improved cycling performance, highlighting the benefits of lithium silting mitigation toward upgraded high-energy Ni-rich cathodes.

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