Machine-Learning-Assisted Screening of Electrolyte Additives for Aqueous Zinc-Ion Batteries via a Molecular...

Additive engineering in aqueous zinc-ion batteries is recognized as a key strategy for improving zinc anode stability. Nevertheless, the conventional trial-and-error screening approach is inefficient, which significantly hinders commercialization progress. This work proposes a descriptor framework-driven strategy integrating machine learning with dual validation from simulations and experiments to enable rapid and precise screening of additives. Through machine learning, we identify the molecular size/volume of electrolyte and electrostatic potential maximum (ESP_max) as the two key descriptors influencing the cumulative capacity (CC) performance, achieving a Pearson correlation coefficient of 0.8707 for the log(CC) prediction. This effectively elucidates the regulatory behavior of additive adsorption on the zinc anode surface toward interfacial water molecules, revealing the mechanism by which the number of interfacial water molecules is modulated, thereby inhibiting the hydrogen evolution reaction. Guided by this model, Potassium L-Aspartate additive (PL-As) is identified as a high-performance additive. Consequently, zinc anode achieves an average coulombic efficiency of 99.86% over 5000 cycles and enables the operation of 0.8 Ah pouch cells. This machine learning-driven descriptor fitting and screening approach establishes a new paradigm for developing high-stability aqueous electrolyte additives.