Spatiotemporally Hierarchical Regulation of Zinc Anode Interface via a Multifunctional Additive for High‐Durability Aqueous Zinc‐Ion Batteries

ABSTRACT The practical deployment of aqueous zinc‐ion batteries is severely hindered by spatiotemporally complex interfacial instabilities at the zinc anode, which cannot be sufficiently addressed by conventional single‐function additives. Here, we present a novel “spatiotemporally hierarchical regulation” strategy that achieves precise, full‐lifecycle intervention in Zn 2+ deposition through a rationally designed multifunctional additive, (3‐amino‐3‐carboxypropyl) dimethylsulfonium chloride (ACDC). Distinct from conventional single‐function additives, ACDC integrates coordinating and electrostatic functionalities within a unified molecular framework, allowing relay‐type regulation across the bulk electrolyte, electric double layer, and electrode interface. This synergistic, multi‐tiered regulation fundamentally reshapes the Zn deposition pathway, enabling stable Zn plating/stripping cycling for over 2100 h at 5 mA cm −2 . Full cells deliver high‐rate capability, suppressed self‐discharge (93% capacity retention after 24 h), and prolonged cycling durability. Meanwhile, the pouch cells exhibit a capacity retention of 84.6% after 100 cycles. Beyond performance enhancement, this work establishes a general molecular design paradigm for spatiotemporal regulation of electrochemical interfaces, offering insights into electrolyte engineering for high‐safety, long‐lifespan aqueous energy storage systems.