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Oxide electrolyte-driven interphase reconfiguration enables durable solid-liquid hybrid lithium batteries
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DOI：10.1016/j.ensm.2026.105451.png)
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Abstract
En 中文
Lithium batteries with Ni-rich cathodes promise high energy density, yet deep delithiation triggers coupled chemo-mechanical degradation, including interfacial reactions, phase reconstruction, and crack propagation. Conventional coatings mainly passivate the outermost surface, leaving lattice instability unresolved. Here we introduce a solid electrolyte-driven interphase reconfiguration strategy by conformally coating LiNi0.8Co0.1Mn0.1O2 (NCM811) with a nanolayer of Li1.3Al0.3Ti1.7(PO4)3 (LATP). Beyond serving as a Li+-conductive, chemically stable surface, LATP releases Al3+ into NCM811 to form an endogenous interphase and a chemo-mechanically reinforced lattice. Al-O multicenter bonding and band hybridization stabilize the lattice-oxygen framework, dynamically buffering oxygen over-oxidation and enabling suppressed oxygen release without structural collapse. Nonmagnetic Al3+ further suppresses Li/Ni cation disorder, improving Li+ transport homogeneity and Ni3+/Ni4+ redox reversibility. Advanced single-particle 3D nano-tomography (TXM nano-CT coupled with spatially resolved XANES) reconstructs particles to correlate valence evolution with morphology, showing suppressed valence heterogeneity and crack-initiating strain localization. Consequently, the interphase-reconfigured NCM811 delivers 402 Wh kg-1 in a Li pouch cell and sustains 1200 cycles in an 8.7 Ah pouch cell paired with a Si-C anode at a lean electrolyte level of 2.0 g Ah⁻¹. This work elevates interface engineering from passivation to an ionically active route for tuning subsurface redox-mechanics coupling in Ni-rich cathodes for high-energy-density batteries.
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