Competitive ion-molecule-coordinated interactions for high-voltage and high-rate lithium batteries under ultra-wide...

The sluggish ion transport and deteriorating electrode-electrolyte interphase hinder the performance of lithium-ion batteries under wide temperature operation, thereby posing substantial challenges in improving both high-voltage and high-rate performance. Herein, the competitive ion-molecule-coordinated interactions (Li⁺-anion-solvent-diluent) achieve a balance that directs an anion-dominated and moderate diluent-interacting solvation structure, resulting in an excellent wide-temperature electrolyte with electrochemical stability up to 5.4 V and high Li-ion conductivity (1.034 mS/cm at -60 °C). The corresponding NCM811||Li cells exhibit capacity retention ratios of 90.74% after 200 cycles at -40 °C and 54.68% for 250 cycles at 70 °C. Additionally, the cell achieves stable cycling performance at a high rate of 10 C at 25 °C. Notably, the assembled NCM811||Graphite pouch battery (3 Ah) can be operated at -106 °C and possesses 2.6 Ah at -30 °C, with 90.28% capacity retention after 90 cycles and stable cycling performance at 50 °C. This work provides a new design principle for electrolyte, which may expedite the development of ultra-wide-temperature lithium-ion batteries.