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Localized Stabilization of Lattice Oxygen in Layered Oxides via Competitive Pathways for Robust Direct Regeneration of Lithium-ion Batteries
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DOI：10.1016/j.ensm.2026.105460.png)
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Abstract
En 中文
LiNixCoyMn1-x-yO2 (0 <x, y < 1, NCM) are indispensable for high-energy-density lithium-ion batteries (LIBs) cathodes, yet the intrinsic instability of lattice oxygen (lattice-O) severely compromises their manufacturing tolerance, high-voltage cyclability, and direct recyclability. Conventional macroscopic stabilization strategies largely fail to account for heterogeneous microscale environments at cathode interfaces, where adverse reactions initiate and propagate, driving localized lattice-O evolution and structural degradation. Here, we systematically investigate lattice-O reactivity in degraded NCM cathodes, focusing on carbon-cathode interfaces as prototypical sites of local heterogeneity. We show that even under globally oxidative conditions, oxygen transport constraints coupled with microscale hot spots at solid-solid contacts generate low-O2 partial pressure and electron-rich microdomains, triggering interfacial reactions governed by local kinetics. To mitigate these degradation pathways, we introduce a competitive oxidation mechanism employing a thermodynamically stronger oxidant than lattice-O within a molten-salt-derived liquid-phase environment, which kinetically redirects interfacial reaction pathways. This strategy suppresses lattice-O migration, preserves the oxygen sublattice, and enables full structural restoration of spent NCM even with Ni content up to 80% cathodes under substantial carbon contamination, achieving near-commercial electrochemical performance. These findings provide a mechanistic framework for understanding and controlling lattice-O stability across the cathode lifecycle.
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