Revealing Surfactant Effect of Trifluoromethylbenzene in Medium‐Concentrated PC Electrolyte for Advanced Lithium‐Ion Batteries

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 (PhCF(3)), 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 PhCF(3), 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, PhCF(3) 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.