Molecular recognition effect enabled by novel crown ether as macrocyclic host towards highly reversible Zn anode

Aqueous Zn 2+ ion batteries present notable advantages, including high abundance, low toxicity, and intrinsic nonflammability. However, they exhibit severe irreversibility due to uncontrolled dendrite growth and corrosion reactions , which limit their practical applications. Inspired by their distinct molecular recognition characteristics, supramolecular crown ethers featuring interior cavity sizes identical to the diameter of Zn 2+ ions were screened as macrocyclic hosts to optimize the Zn 2+ coordination environment, facilitating the suppression of the reactivity of H 2 O molecules and inducing the in-situ formation of organic–inorganic hybrid dual-protective interphase. The in-situ assembled interphase confers the system with an “ion-sieving” effect to repel H 2 O molecules and facilitate rapid Zn 2+ transport, enabling the suppression of side reactions and uniform deposition of Zn 2+ ions. Consequently, we were able to achieve dendrite-free Zn 2+ plating/stripping at 98.4% Coulombic efficiency for approximately 300 cycles in Zn||Cu cell, steady charge–discharge for 1360 h in Zn||Zn symmetric cell, and improved cyclability of 70% retention for 200 cycles in Zn||LMO full cell, outlining a promising strategy to challenge lithium-ion batteries in low-cost, and large-scale applications.