Molecule Design for Non‐Aqueous Wide‐Temperature Electrolytes via the Intelligentized Screening Method

Abstract Operating a lithium‐ion battery (LIB) in a wide temperature range is essential for ensuring a stable electricity supply amidst fluctuating temperatures caused by climate or terrain changes. Electrolyte plays a pivotal role in determining the temperature durability of batteries. However, specialized electrolytes designed for either low or high temperatures typically possess distinct features. Therefore, wide‐temperature electrolytes (WTEs) are necessary as they encompass a combination of diverse properties, which complicates the clear instruction of WTE design. Here we represent an artificial intelligence (Al)‐assisted workflow of WTE design through stepwise parameterizations and calculations. Linear mono‐nitriles are identified as ideal wide‐liquidus‐range solvents that can “softly” solvate lithium ions by weak interactions. In addition, the explainable modules revealed the halogenoid similarity of cyanide as fluorine on the electrolyte properties (e.g. boiling point and dielectric constant). With the further introduction of an ether bond, 3‐methoxypropionitrile (MPN) has been eventually determined as a main electrolyte solvent, enabling the battery operation from −60 to 120 °C. Particularly, a LiCoO 2 /Li cell using the proposed WTE can realize stable cycling with capacity retention reaching 72.3 % after 50 cycles under a high temperature of 100 °C.