In situ supramolecular coating breaking the trade-off between anticorrosion and ion conduction for stable zinc anode

Aqueous Zn-ion batteries (ZIBs) have emerged as promising candidates for next-generation energy storage due to their inherent safety and cost-effectiveness. However, rampant dendrite growth and corrosive side reactions at the zinc metal anode severely compromise cycling stability. While artificial coatings show potential in addressing these issues, existing strategies struggle to reconcile the conflicting requirements of robust corrosion resistance and efficient Zn²⁺ transport. Herein, we present a dynamic interface engineering approach through in situ supramolecular self-assembly of an amino-silicone oil (ASO) to solve this contradiction. Enabled by a fluorinated azeotropic solvent system, the ASO coating spontaneously reorganizes into a supramolecular coating upon contact with aqueous electrolyte through Zn²⁺ coordination. This self-assembled structure establishes dual functionalities: a hydrophobic polydimethylsiloxane matrix suppressing water-induced corrosion, and amino-rich domains enabling spatially confined ion transport. Consequently, the ASO-coated Zn anode (ASO-Zn) achieves ultra-stable cycling over 1800 h and much low overpotentials of 40 and 78 mV at 1 and 10 mA cm⁻², respectively. When matched with MnO₂ cathodes, the ASO-Zn||MnO₂ full cells exhibit exceptional rate performance and cycling stability. This work pioneers a solvent-guided supramolecular assembly strategy that dynamically regulates interfacial chemistry, providing a universal paradigm for metal anode protection in aqueous batteries.