Successive Gradient Internal Electric Field Strategy Toward Dendrite‐Free Zinc Metal Anode

Abstract With the rapidly increasing demand for grid‐scale energy storage systems, rechargeable aqueous zinc ion batteries (ZIBs) are capturing attention as a highly promising technology with low cost and high safety. Nevertheless, rampant dendrite growth, hydrogen evolution reaction (HER), and corrosion of the zinc anode have dramatically impacted their practical application. Here, a self‐supported modified layer with ultrafine high‐entropy nanoparticles (2 nm) as the zincophilic sites is realized to modify the Zn anode for the first time. High‐entropy materials with unique continuously distributed potential gaps significantly reduce the activation energy of multi‐electron reactions and modulate ion transport during zinc deposition. Moreover, thanks to the hydrophobic properties and effective desolventizing ability of the ultrafine high‐entropy nanomaterial, the unfavorable side reactions of the zinc anode are prevented to promote the zinc deposition process. As a result, stable cycling of 3500 h at 1 mA cm −2 and 600 h at a high current density of 10 mA cm −2 is achieved. Coin cells and flexible pouch cells assembled with KMO and NH 4 V 4 O 10 cathodes also demonstrate promoted electrochemical performance. The dual effects of accelerating and homogenizing mechanisms in high‐entropy materials provide a new strategy for stabilizing zinc metal anodes.