High Entropy Oxides Modulate Atomic‐Level Interactions for High‐Performance Aqueous Zinc‐Ion Batteries

Abstract The strong electrostatic interaction between high‐charge‐density zinc ions (112 C mm −3 ) and the fixed crystallinity of traditional oxide cathodes with delayed charge compensation hinders the development of high‐performance aqueous zinc‐ion batteries (AZIBs). Herein, to intrinsically promote electron transfer efficiency and improve lattice tolerance, a revolutionary family of high‐entropy oxides (HEOs) materials with multipath electron transfer and remarkable structural stability as cathodes for AZIBs is proposed. Benefiting from the unique “cock‐tail” effect, the interaction of diverse type metal‐atoms in HEOs achieves essentially broadened d ‐band and lower degeneracy than monometallic oxides, which contribute to convenient electron transfer and one of the best rate‐performances (136.2 mAh g −1 at 10.0 A g −1 ) in AZIBs. In addition, the intense lattice strain field of HEOs is highly tolerant to the electrostatic repulsion of high‐charge‐density Zn 2+ , leading to the outstanding cycling stability in AZIBs. Moreover, the super selectability of elements in HEOs exhibits significant potential for AZIBs.