Lithium metal anodes promise ultra-high energy densities (>500 Wh/kg) but suffer from dendrite growth and low Coulombic efficiency (<80%). Recent studies have shown that electrolyte additives like LiNO3 and CsPF6 can improve Coulombic efficiency to >99% by forming stable solid-electrolyte interphases (SEIs). For instance, LiNO3 forms a dense SEI layer rich in Li3N (ionic conductivity ~10^-4 S/cm), which suppresses dendrite formation even at current densities >5 mA/cm^2.
Additives such as fluoroethylene carbonate (FEC) have been shown to enhance SEI stability by increasing its mechanical strength (>1 GPa) and reducing its thickness (<50 nm). This results in improved cycling performance with over 200 cycles at >99% efficiency for lithium metal batteries (LMBs). Additionally, FEC reduces electrolyte decomposition by forming a protective layer on the anode surface, decreasing gas evolution by ~70%.
Recent research has explored synergistic effects of dual additives like LiNO3 + CsPF6 or FEC + vinylene carbonate (VC). These combinations have demonstrated unprecedented improvements in cycle life (>500 cycles) and rate capability (>3C). For example, VC forms a polymerized SEI layer that enhances mechanical flexibility while maintaining high ionic conductivity (~10^-5 S/cm). This dual-additive approach has been particularly effective in high-concentration electrolytes (>4 M LiFSI), where it further stabilizes the electrolyte-anode interface.
The development of advanced characterization techniques like cryo-electron microscopy (cryo-EM) has enabled atomic-level insights into SEI formation mechanisms induced by additives. These studies reveal that additives like CsPF6 promote uniform lithium deposition by creating a gradient concentration field near the anode surface. This understanding is critical for designing next-generation additives tailored for LMBs operating under extreme conditions (>5 mA/cm^2).
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