Zinc‐Seeded PEDOT:PSS Aerogel Host as Highly Reversible Dendrite‐Free Zinc Metal Anode

Abstract The parasitic reactions and rampant dendrite growth on the Zn anode side pose significant obstacles to the future applications of aqueous zinc ion batteries. Herein, a lightweight anode host is reported by introducing nanosized metallic Zn into the poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) (P‐S) aerogel (Zn/P‐S). The ‒SO₃H groups interact with Zn²⁺ and guild their migrations along PSS chains, while the nanosized Zn offer additional nucleation sites and homogenize the electrical and Zn²⁺ ion concentration. Owing to these synergistic effects, uniform and dense Zn deposition with the (002) plane aligned parallel to the P‐S substrate is achieved, even at a high plating capacity of 20 mAh cm⁻². Moreover, the deposited Zn over the Zn/P‐S host (Zn@Zn/P‐S) exhibits a highly reversible plating/stripping behavior with Coulombic efficiency maintained at 99% over 700 cycles. Consequently, the Zn@Zn/P‐S‐based symmetric Zn||Zn cell can work stably over 500 h at 0.5 mAh cm^‒2 and 100 h at 4 mAh cm^‒2 with a depth of discharge of 40%. A Zn@Zn/P‐S||NaV₃O₈ full battery presents a high rate capability along with 82.2% capacity retention after 1000 cycles at 2 A g^‒1. This strategy provides a novel approach for designing polymer‐based Zn anodes with corrosion‐resistant and dendrite‐free striping/plating behaviors.