Solvent Anchored Electrolytes for Lithium‐Ion Batteries Working at High Voltage and Wide Temperature

Lithium-ion batteries (LIBs) suffer from severe performance fading under coupled conditions of high voltage and wide temperature because cold retards Li+ migration and desolvation kinetics while heat or high voltage exacerbates parasitic reactions and electrode destabilization. Herein, we propose a solvent-anchored paradigm for electrolyte design via electrostatic potential matching to enable stable battery operation across the demanding voltage-temperature matrix. The fine-tuned electrolyte, which is composed of well-matched dimethyltrifluoroacetamide solvent and fluorotoluene diluent, features a site-specific solvation structure with anion-dominated inner shell and solvent-anchored outer cluster. This unique configuration facilitates fast Li+ desolvation and robust interphase formation on both the lithium/graphite anode and LiCoO2 cathode. Remarkably, the formulated electrolyte enables stable operation of graphite||LiCoO2 full cells up to a charging voltage of 4.5 V from -60°C to 80°C, indicating its promising applicability to fortify LIB performance under harsh conditions.