Modulating Lattice Oxygen and Transport Kinetics of Li-Rich Cathodes in All-Solid-State Batteries Through Multifunctional Li3ScF6 Protective Layer
Corresponding Author: Li‑Zhen Fan
Nano-Micro Letters,
Vol. 18 (2026), Article Number: 383
Abstract
Li-rich Mn-based oxide (LRMO) cathodes represent promising candidates for high-energy-density all-solid-state lithium batteries (ASSLBs). Nonetheless, irreversible oxygen release and sluggish transport kinetics result in faded voltage and degraded cycling stability, severely impeding their practical applications in ASSLBs. Herein, a high-quality artificial interface layer was constructed on the LRMO surface via a facile sol–gel method followed by thermal treatment, yielding a Li3ScF6 protective layer comprising a Li3ScF6 surface coating region and a subsurface Sc doping region. Specifically, Li3ScF6 surface coating effectively suppresses continuous interfacial side reactions between the cathode and solid electrolyte, thereby improving interfacial transport kinetics; the strong Sc–O bond stabilizes the lattice oxygen framework and inhibits oxygen release, thereby enhancing the reversibility of the oxygen redox reaction. Consequently, the ASSLBs with the modified LRMO cathode exhibit remarkable fast-charging capability (136.8 mAh g−1 at 1.0 C) and excellent capacity retention (83.9% after 500 cycles at 0.3 C). In addition, the ASSLBs achieve outstanding long-term cycling stability at a high areal capacity of 4.17 mAh cm−2, retaining 81.8% of its capacity after 300 cycles at 60 °C. This study offers new insights into the rational design of high-capacity and high-voltage LRMO cathode materials for high-energy-density ASSLBs.
Highlights:
1 A multifunctional Li3ScF6 protective layer is engineered to simultaneously modulate lattice oxygen stability and interfacial transport kinetics of Li-rich cathodes in all-solid-state batteries.
2 The Li3ScF6 layer significantly enhances interfacial contact between Li-rich Mn based oxide and the solid electrolyte, suppressing parasitic interfacial reactions and facilitating faster Li+ transport across the interface. Concurrently, the strong Sc–O bonding stabilizes the lattice oxygen framework, suppresses oxygen evolution, and improves the reversibility of oxygen-anion redox.
3 The well-configured cells exhibit outstanding electrochemical performance, enabling fast charging, long-term cycling stability, and stable operation at high areal capacities in all-solid-state batteries.
Keywords
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