A Quantitative Electrostatic Potential Descriptor Enables Deep Learning-Accelerated Discovery of High-Performance Lithium-Ion Battery Electrolytes.

Abstract

Rational electrolyte design for high-energy-density lithium-ion batteries (LIBs) urgently demands precise and quantitative molecular descriptors of solvation power to enable deep learning (DL)-accelerated screening, yet such descriptors remain lacking. Here, we introduce the electrostatic potential ratio |ESPmin|/ESPmax (ESPratio) as a quantitative descriptor capturing the balance between electron-donating and electron-accepting capacities, and identify a solvation modulation zone (0.9 < ESPratio < 2.4) through unsupervised clustering of 344 molecules encompassing 196 experimentally reported LIB electrolyte molecules. By combining this descriptor with self-supervised pre-trained DL models fine-tuned on small experimental datasets, we enable hierarchical screening of ∼106 PubChem molecules and prioritize electrolyte candidates from previously unexplored chemical space. Experimental evaluation of representative candidates, including TBDN and PIV as co-solvents and additional nitrile-containing molecules as electrolyte additives, confirms that the ESPratio-guided workflow can enrich chemically meaningful electrolyte candidates for high-voltage Li||LiCoO2.