Liquified SO2 induced solid/cathode electrolyte interphase for lithium ion batteries

Abstract

Formation of robust solid/cathode electrolyte interphases (S/CEI) is vital for long-term stability and high-performance operation of lithium-ion batteries (LIBs), particularly under high voltage regimes. However, engineering electrochemically stable S/CEIs that effectively suppress interfacial side reactions remains a key challenge. Herein, we introduce a liquefied sulfur dioxide (SO2)– ionic liquid complex as a fluorine-free multifunctional electrolyte additive for the first time that significantly improves the formation of sulfate/sulfite-rich S/CEI layers at both graphite and NMC811 interfaces. The unique SO2-N coordination with a 1,2,4-triazolide-based ionic liquid enables homogeneous SO2 dissolution, resulting in controlled SO2 decomposition during the initial electrochemical cycle. This decomposition yields sulfur-rich interphase species that stabilize the electrolyte-electrode interface, reduce impedance growth, and lessen electrolyte decomposition. Electrochemical tests show significantly improved cycle life, reduced polarization, and increased Coulombic efficiency for both anodes and cathodes. XPS confirms the presence of SO2-derived surface species that contribute to interfacial stability. This approach highlights a new direction for interphase engineering using liquefied gas additives and opens pathways for sulfur-based S/CEI chemistry in advanced battery systems.