Abstract:

Lithium-ion batteries are approaching their theoretical energy density limits, struggling to meet the escalating demands of modern energy storage and power applications, particularly for electric vehicles. Lithium metal batteries (LMBs) offer a higher energy density alternative, yet their potential is hindered by unstable electrolyte/electrode interfaces, which significantly curtail their lifespan. To address these challenges, this study employed Polyfluoric acid (PFC) as an electrolyte additive that regulates solvent-Li+ coordination dynamics. This intervention enables rapid lithium-ion transport while guiding uniform lithium depositing/stripping on the metal anode, achieving stable cycling over 1,000 hours under high current density (10 mA cm⁻²/10 mAh cm⁻²) with demonstrated flame-retardant capabilities. Notably, while recent research prioritizes solid-state lithium metal batteries, their complex synthesis processes and compromised ionic conductivity. Drawing inspiration from liquid-phase polymerization mechanisms, our strategy utilizes PFC to protonate solvent molecules, inducing spontaneous liquid-to-solid phase transformation. This approach simultaneously handles interfacial stability and ionic transport limitations, enabling high-rate cycling (1C) in full-cell configurations with LiFePO₄ cathodes while maintaining 90% capacity retention over 500 cycles. The developed methodology establishes a multifunctional electrolyte design paradigm applicable to liquid-solid hybrid systems, with demonstrated compatibility extending to silicon-based batteries.

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