Synergistic Interfacial‐Bulk Solvation Enables Fast‐Charging and Low Temperature Li‐Ion Batteries

Abstract The performance degradation of lithium‐ion batteries under low‐temperature conditions originates from critically retarded bulk solvation dynamics, kinetically hindered interfacial desolvation barriers, and unstable electrode‐electrolyte interfaces. This work proposes a synergistic interfacial‐bulk solvation regulation strategy that fundamentally reconstructs electrolyte microenvironments to establish an anion‐rich solvation structure. This approach simultaneously enhances bulk ion conductivity through optimized Li + ‐anion coordination networks and facilitates anion incorporation into the solvation sheath, dramatically reducing the Li + desolvation energy barrier, while constructing low‐resistance anion‐derived inorganic‐rich films. With this electrolyte, the graphite/ LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) full cell delivers 108.2 mAh g −1 at 5C (25 °C), demonstrating excellent rate performance, and maintains 94.1% capacity retention after 300 cycles under 2C cycling. Notably, the system remains functional even at −70 °C, exhibiting exceptional cryogenic performance. This work provides reference designs and critical theoretical guidance for developing advanced low‐temperature electrolytes.