Superhydrophobic and Highly Flexible Artificial Solid Electrolyte Interphase Inspired by Lotus Effect Toward Highly Stable Zn Anode

Abstract Due to their cost‐effectiveness, high safety, and environmental friendliness, aqueous zinc‐ion batteries (AZIBs) are among the most promising technologies for next‐generation energy storage systems. Nonetheless, dendrite growth, hydrogen evolution, and corrosion at zinc (Zn) anode severely hinder their practical application. In this study, a combination of molecular self‐assembly engineering, squeegee coating, and air spraying process is employed to create a superhydrophobic and highly flexible artificial solid‐electrolyte‐interface layer on Zn anode (denoted as SFM/Zn). Self‐assembled monolayer of triethoxy‐3‐aminopropylsilane optimizes Zn 2+ migration kinetics. The superhydrophobic interface, formed by polydimethylsiloxane (PDMS) and trimethoxy(octadecyl)silane (OTS)‐modified nanosilicon dioxide particles, inhibits water‐related side reactions. Furthermore, the highly flexible PDMS serves as a dynamic adaptive interface for Zn anode, effectively alleviating the “tip effect”. Consequently, the SFM/Zn||SFM/Zn symmetrical cells enable reversible and stable Zn plating/stripping at both ultralow current density (0.2 mA cm −2 ) and ultrahigh current density (45 mA cm −2 ). The assembled Zn‐vanadium (SFM/Zn||NH 4 V 4 O 10 ) cell deliver stable average Coulombic efficiency (nearly 100%) and ultralong cycling stability (135.5 mAh g −1 after 500 cycles at 5 A g −1 and 173.2 mAh g −1 after 1000 cycles at 2 A g −1 ). This innovative superhydrophobic three‐layered strategy sheds new light on designing highly durable Zn anode for high‐performance AZIBs.