Despite wide-temperature tolerance and high-voltage compatibility, employing propylene carbonate (PC) as electrolyte in lithium-ion batteries (LIBs) is hampered by solvent co-intercalation and graphite exfoliation due to incompetent solvent-derived solid electrolyte interphase (SEI). Herein, trifluoromethylbenzene (PhCF3 ), featuring both specific adsorption and anion attraction, is utilized to regulate the interfacial behaviors and construct anion-induced SEI at low Li salts' concentration (<1 m). The adsorbed PhCF3 , showing surfactant effect on graphite surface, induces preferential accumulation and facilitated decomposition of bis(fluorosulfonyl)imide anions (FSI- ) based on the adsorption-attraction-reduction mechanism. As a result, PhCF3 successfully ameliorates graphite exfoliation-induced cell failure in PC-based electrolyte and enables the practical operation of NCM613/graphite pouch cell with high reversibility at 4.35 V (96% capacity retention over 300 cycles at 0.5 C). This work constructs stable anion-derived SEI at low concentration of Li salt by regulating anions-co-solvents interaction and electrode/electrolyte interfacial chemistries.
Keywords: adsorption; electrolytes; lithium-ion batteries; solid electrolyte interface; solvation structure.
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