Enhanced Redox Electrocatalysis in High-Entropy Perovskite Fluorides by Tailoring d–p Hybridization

Abstract

Highlights The tailored KCoMnNiMgZnF3-HEC cathode delivers extremely high discharge capacity (22,104 mAh g−1), outstanding long-term cyclability (over 500 h), preceding majority of traditional catalysts reported. Entropy effect of multiple sites in KCoMnNiMgZnF3-HEC engenders appropriate regulation of 3d orbital structure, leading to a moderate hybridization with the p orbital of key intermediate. The homogeneous nucleation of Li2O2 is achieved on multiple cation site, contributing to effective mass transfer at the three-phase interface, and thus, the reversibility of O2/Li2O2 conversion.

Keywords

• Lithium–oxygen batteries
• KCoMnNiMgZnF3-HEC perovskite fluoride
• Entropy effect
• Catalytic kinetics
• d–p orbital hybridization