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Electronically Coupled Interface Stabilizes Deeply Delithiated Surfaces of Single-Crystalline Ni-Rich Cathodes
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DOI：10.1016/j.ensm.2026.105455.png)
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Abstract
En 中文
Single-crystalline Ni-rich layered oxides offer a promising route to high-energy lithium-ion batteries, yet their high-voltage durability remains limited by the intrinsically reactive surface formed under deep delithiation. Highly oxidized transition-metal–oxygen units and oxygen-hole-like lattice states can electronically couple with electrolyte molecules, initiating parasitic interfacial reaction and creating Li+ diffusion barrier. Here we report an ultrathin cyclized polyacrylonitrile (cPAN) interphase that stabilizes single-crystalline LiNi0.83Co0.12Mn0.05O2 by electronically buffering the deeply delithiated cathode surface. The nitrogen-containing conjugated framework couples electronically with the Ni-rich surface, reshaping the surface electrostatic potential and shifting the valence-band edge away from the Fermi level. The resulting chemically buffering interphase weakens parasitic charge transfer from carbonate electrolyte molecules to unoccupied Ni 3d–O 2p hybridized states, while preserving the interfacial charge-transfer kinetics required for reversible cathode redox. As a result, the optimized SC-NCM83@cPAN cathode achieves an initial Coulombic efficiency of 92% and retains 90% of its initial capacity after 200 cycles at 1 C and 45°C between 2.7 and 4.5 V. Our results highlight electronically coupled polymeric interphases as a generalizable route to engineer electrochemical interfaces in high-energy Ni-rich cathodes.
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