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 Zn²⁺, leading to the outstanding cycling stability in AZIBs. Moreover, the super selectability of elements in HEOs exhibits significant potential for AZIBs.