High‐Entropy‐Inspired Multicomponent Electrical Double Layer Structure Design for Stable Zinc Metal Anodes

Abstract Regulating the electrical double layer (EDL) structure can enhance the cycling stability of Zn metal anodes, however, the effectiveness of this strategy is significantly limited by individual additives. Inspired by the high‐entropy (HE) concept, we developed a multicomponent (MC) EDL structure composed of La 3+ , Cl − , and BBI anions by adding dibenzenesulfonimide (BBI) and LaCl 3 additives into ZnSO 4 electrolytes (BBI/LaCl 3 /ZnSO 4 ). Specifically, La 3+ ions accumulate within EDL to shield the net charges on the Zn surface, allowing more BBI anions and Cl − ions to enter this region. Consequently, this unique MC EDL enables Zn anodes to simultaneously achieve uniform electric field, robust SEI layer, and balanced reaction kinetics. Moreover, the synergistic parameter – a novel descriptor for quantifying collaborative improvement – was first proposed to demonstrates the synergistic effect between BBI and LaCl 3 additives. Benefitting from these advantages, Zn metal anodes achieved a high reversibility of 99.5 % at a depth of discharge (DoD) of 51.3 %, and Zn|MnO 2 pouch cells exhibited a stable cycle life of 100 cycles at a low N/P ratio of 2.9.