A Synergistic Zincophilic and Hydrophobic Supramolecule Shielding Layer for Actualizing Long‐Term Zinc‐Ion Batteries

The dimethoxypillar[5]arene (DP[5]) supramolecule, featuring synergistic zincophilic and hydrophobic characteristics, is engineered as an anode shielding layer to suppress side reactions and dendrite formation, thereby significantly prolonging the lifespan of Zn-ion batteries.

Abstract

The zinc metal anodes are liable to experience detrimental dendrite growth and side reactions, thereby limiting the lifespan of aqueous Zn-ion batteries. Here, a readily available supramolecule, dimethoxypillar[5]arene (DP[5]), is utilized as a shielding layer to stabilize the Zn anode by exploiting its zincophilicity derived from the ─OCH₃ functional groups and its hydrophobicity from the hydrophobic backbone. The DP[5] shielding layer regulates the solvation sheath of Zn²⁺ and facilitates uniform zinc deposition. Swelling and dendrite formation are obviously suppressed in both the symmetric and full cells. The DP[5]-Zn symmetrical cell cycles stably for 5500 h, and achieves a coulombic efficiency of 99.76% in a DP[5]-Zn||Cu half-cell after 2200 cycles. The DP[5]-Zn||V₂O₅ full cell maintains 92.03% of initial capacity after 6000 cycles. Given the cost-effective fabrication and environmental friendliness of DP[5] films, this material may pave the way for practical applications of zinc anodes.