Synergistic Static and Dynamic Interfacial Regulation Toward Robust Zinc Batteries

Abstract

ABSTRACT Aqueous zinc (Zn) metal batteries (AZMBs) are promising for sustainable energy storage, yet their development is severely compromised by the interfacial instability arising from a water‐rich and disordered electric double layer (EDL). Herein, we establish a rational screening strategy that combines density functional theory with molecular dynamics simulations to identify cationic regulators (both organic and inorganic) capable of reshaping the EDL structure through optimized interfacial affinity and transport kinetics. The results reveal that 1‐ethyl‐3‐methylimidazolium exhibits strong interfacial affinity, which enables the formation of a hydrophobic shielding layer that suppresses parasitic reactions, demonstrating a “static passivation” effect. In contrast, sodium ion, as electric field‐responsive species, provides “dynamic regulation” by homogenizing Zn 2+ flux and lowering the desolvation energy barrier. Consequently, this dual‐cation strategy constructs a water‐poor and ordered EDL, enabling Zn anodes to operate stably for over 5000 h with a high Coulombic efficiency of 99.73%. Ultimately, guided by these mechanistic insights, a machine learning framework is further developed to enable predictive and scalable additive screening.